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Optics and Spin Photonics of Metallic Nanostructures Jean-Yves Bigot

Institut de Physique et Chimie des Matriaux de Strasbourg

Universit de Strasbourg - CNRS -

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1. The static optical and magneto-optical properties of metallic nanoparticles


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

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

Reflection

Transmission

Glass containing Au and Ag nanoparticles


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.

Rose window from Strasbourg Cathedral (15 m diameter)

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

Au nanoparticles as agent for high contrast imaging


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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Nanoparticles as catalysts for controlling reactions


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

Generalized reaction coordinate

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

Self organization of nanoparticles


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

3D supra crystals of Cobalt nano-particules

Collaboration : LM2N - Universit Pierre et Marie Curie Paris ; (I. Lisiecki, C. Petit, M.-P. Pilni)
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Seoul - 2009 - Jean-Yves Bigot - Winter_school_IPCMS-QMMRC

A historical note about Nanosciences

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

M PC

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

1. The static optical and magneto-optical properties of metallic nanoparticles


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

M PC

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

Intuitive approach to the response function of metallic nanoparticles


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

+ + + +

Pind = ( eff 0 ) E ; E loc

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

Pind = 0E + 3 0

The effective dielectric function eff is given by :

( 0 ) eff = 0 + 3N 0 ( + 2 0 )
y s n e d l a i t p O c

Resonance if :

e ( ) = 2 0

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

e ( ) = 2 0

For metals : () and Re() < 0 . Example Drude model of electrons:


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

surface plasmon resonance

0.5

- 20 -5
-10

= p
10 12

0.0

h (eV)
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e [ ( )] = 2 0

h (eV)

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

Absorption spectra of assemblies of Silver, Gold and Copper metallic nanoparticles

1.0 Absorption (normalized) 0.8 0.6 0.4 0.2 0.0 300

Au Ag Cu

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

400

500

600

700

Wavelength (nm)

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Au - Ag bimetallic alloys of nanoparticles

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

0.1 0.2 0.4 0.5 0.6 1

414 428 466 475 486 525

29 27 32 26 26 44

12 2 7 13 17 28

2098 1583 2156 2249 1989 1997

482 502 554 584 600 600

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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 ?

Needs for comprehensive understanding of metallic nano-objects

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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

p : Plasmon frequency (~10 eV) : damping !!!

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

-m (1/D) max for = p Excitation spectrum

Optical absorption
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What is missing in the Drude model ?

Dispersion : (q) Temperature of electrons: (, q, kbT) Interband transitions

Calculation of dielectric function for excitation by electromagnetic field

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

< kl = 1/ 2u kl (r)e ikr Bloch functions with lattice periodicity


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In first order perturbation one gets :

ih

kl 1 k + q, l ' t

= ( Ekl Ek + q ,l ' ) kl 1 k + q, l ' + [ f o ( Ek + q ,l ' ) f o ( Ekl )] kl H int (r, t ) k + q, l '

e with : kl H int (r, t ) k + q, l ' = kl p.A(q, t )eiqr k + q, l ' mc


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 )]

e kl p.A(q)eiqr k + q, l ' mc ih h Ek + q ,l ' + Ekl

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Current density operator J(q) :

e 1 e 0 J (q ) = Tr exp(iqr ) A(q) Tr exp(iqr ) p mc m


Diamagnetic response Paramagnetic response

Using the response theory : Ohms law

J ( q, ) =

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

One finally obtains the Transverse dielectric function:

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

k ,l ,l '

kl p k + q, l '

f o ( Ek + q ,l ' ) f o ( Ekl ) Ek + q ,l ' Ekl h + ih

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

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

l = p band Fermi level EF

E intraband transition !

interband transition
kl p k + q, l '
2

f o ( Ek + q ,l ' ) f o ( Ekl ) Ek + q ,l ' Ekl h + ih

l = d band

For photons q ~ 0 (as compared to Brillouin Zone)

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

Excitation spectrum of quasi-particles (l=l)

( 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

Landau damping : decay of plasmons into quasiparticles

From longitudinal dielectric function

h =

Re() = 0

h 2 (q 2qk F ) 2m

2kF
Fermi surfaces of radius kF kF+q

Momentum space accessible for quasiparticles excitations


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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 '

m: effective mass of electrons in corresponding band

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

Reason for the different absorption of the transition metal nanoparticles

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

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

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Inhomogeneous systems and Dielectric confinement


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

Fourier transform of Maxwell equations


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

Helmoltz equations :
: dielectric function inside or outside the sphere

q0 =

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

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

Search solutions like : =R(r)()() Transmitted waves: 1 e r t = 2 cl l (kr)Pl( 1 )( cos ) cos k l =1

(a) (b)

r tm

2 = 2 0 2 k ( 2 )

d l l (kr)Pl( 1 )( cos ) sin


l =1

Scattered waves: 1 e r d = 2 al l(k d r)Pl ( 1 )( cos ) cos k d l =1

(a) (b)

2 r = 2 0 2 k d ( 2)
m d
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bl l(k d r)Pl ( 1 )( cos ) sin


l =1

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

Using the flux of energy per unit time :


S = c Re E H 8

W=

sphere

S ds

One obtains the cross sections of extinction and scattering


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

2 2 n d l +1 x 2l +1 n 2 nd l a l i 2 l [1.3.5...( 2l 1 )]2 n 2 l + 1 n 2 d l 2 n d l +3 x 2l +3 l 2 (n 2 n d ) bl i l(l + 1 )( 2l + 1 )( 2l + 3 )[1.3.5...( 2l 1 )]2

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

Mie scattering of Metallic nanoparticles


(u.a)

0.6

d=50nm,lmax=1 d=50nm,lmax=5 d=50nm,lmax=7

0.4

d=70nm,lmax=1 d=70nm,lmax=5 d=70nm,lmax=7

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)

Rule of thumb: First order is OK up to diameter ~/10

2 2 1 1 0

Copper

-1

2.0 2.5 nergie (eV)

3.0

2.0

nergie (eV)

2.5

3.0

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In chapter 2 we will discuss the damping parameter

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

1. The static optical and magneto-optical properties of metallic nanoparticles


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

Performances in Spintronics devices


Tunnel Magneto Resistance

R
MRT = R

R
R

Perpendicular recording MRAM from TOSHIBA

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)

Explore new approaches : Spin Photonics ?


S

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

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

1 Terabits/inch2; 10 GHz 10 THz


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

Associate Ultrafast Optics with Magnetism


-20 10 0 20
50

M (u.a)

-50x10

-6

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-10

How fast and how short ?

Basic principles of magneto-optics

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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Illustration of Faraday rotation and ellipticity

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-

Linearly polarized light

Linearly rotated Kerr magneto-optical configurations


(j,k) : sample plane

elliptic non-rotated

k j
b ent ncid I eam

M
Re

fle cte d

(i,j) : plane of incidence


Polar : M // i ; Longitudinal : M // j ; Transverse : M // k
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An easy way to understand Magneto-optics !

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

with : p2 = Ne2/m0 and = eB0 /m


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Generalized magneto-optical response


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

2 4ci x M (r, ) xx E(r, ) = - 2 E(r, ) + 4P(r, ) + c


P (r, ) = P L (r, ) + P NL (r, ) M (r, ) = M L (r, ) + M NL (r, )
Linear :
(1) Pi(1) () = ij () E j () j

Non magnetic response Magneto-optical response

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

Nonlinear (third order) :


jkl

Coupling with field H

(3) Pi(3) () = ijkl (; 1 , 2 , 3 ) E j (1 )E k ( 2 )E l ( 3 ) with = 1 + 2 + 3

(3)MO M i(3) () = ijkl (; 1 , 2 , 3 ) E j (1 )E k (2 )E l (3 ) ; = 1 + 2 + 3 jkl

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A less easy way to understand Magneto-optics !


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

Pn2 h Pn = + V(rn ) + s V(rn ) + Veff (rn ) 2 2 n 2m n 4m n c


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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The light matter interaction is treated semi-classically

H Rn =

e n A light (rn ) 2 mnc

Amag(rn) : vector potential of the applied light field

n = Pn + s n V(rn )

s n V(rn )

Spin orbit coupling sn : Pauli spin operator

Careful ! this is a pure 1/c2 relativistic interaction term !

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Total absorbed energy :

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

, : energy levels of the electronic system

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 or = +, -) are the components of the generalized momentum. By definition :

= ( 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

- +

Transition probability elements

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

Louis Nel 1949 :

2 KV

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KV (1 H / H K ) 2 k BT

with : H K =

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

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

0 (P) W.F. Brown 1959 Langevin model


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P : Damping of the precession (frequency p)

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Langevin approach to magnetization dynamics: Brown 1963


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
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Incoherent term

Cobalt nanoparticles : ion implantation in dielectric matrices (Si02 and Al203)


C. DOrlans, C. Estourns

Spherical monodomain particles


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. Ultrafast laser optics of metals


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

Evib ~ 10-2 eV Tvib ~ 100 fs

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Probing transition states : The case of NaI (A. Zewail et al.)

A. Zewail, 1999 Nobel price in chemistry for his studies of the transition states of chemical reactions using femtosecond spectroscopy
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Wave-packet dynamics associated to C=C vibrations of Polydiacetylene


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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Quantum Beats between excitons


Appl. Phys. Lett., 87, 192104 (2005)
E1

Piezoelectric CdTe QW
HH1 HH2

e1h1 and e1h2 excitons sharing a common conduction band level

2.5

2.0

retard (ps)

1.5

1.0

0.5

2.5 2.0 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

M PC

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

s) (p

) (nm

(nm)

Femtosecond isomerization in retinal proteins


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

M PC

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

* 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

But there is more than just temporal considerations !


M PC S

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

Time versus frequency domains

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

A coherent white light source !


I M PC S

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

Density of electromagnetic field


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

M PC

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

One photon excitation : h

Two-photon excitation : 2x(h/2)

fluorescence

fluorescence

h/2
S

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

M PC

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

Ablation of matter by lattice heating versus electron plasma

Nanosecond

Femtosecond

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

M PC

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

Self phase modulation : generation of white light continuum

Kerr nonlinear index Phase of propagating laser pulse Instantaneous frequency

n = n 0 + n 2 I(t) + ... z (t) = n 2 I(t) c z dI(t) d(t) (t) = = n2 dt c dt

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

M PC

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

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

1016-1020 W/cm2 : Relativistic plasma physics

M PC

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

2. Ultrafast laser optics of metals


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. .

M PC

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

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

k ,l ,l '

kl p k + q, l '

f o ( Ek + q ,l ' ) f o ( Ekl ) Ek + q ,l ' Ekl h + ih

* 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.
I M PC S

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

Screened Coulomb Interaction between quasi-particles

i
W( r,r; Ei Ef )

f E Fermi
Conduction electrons

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

Vq : Fourier transform of Coulomb interaction


requires a model for (q, )
Random Phase Approximation (RPA) or (q, ) = RPA(q, ) G(q, )(RPA(q, ) -1) (G : local field factor)
I M PC S

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

Alternatively: 1. Fermi liquid approach


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)

M PC

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

Schematic of relaxation in a metal excited with (t) pulse


(E)

simple metal : Fermi-Dirac ( E,Te )

athermal Distribution

Electronic dephasing : t < 20 fs plasma oscillations


EF

(E)

Fermi-Dirac Hot : T ~ 1000 K


3

Thermalization of electrons: t < 200 fs diffusion between quasi-particles (Coulomb interaction)

(E)

Cooling of electrons and Heating of lattice : t < 5 ps (electrons-phonons interaction)


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

Fermi-Dirac T > 300 K

EF
M PC S

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

Electron-lattice relaxation: two-temperatures model


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

C e (T e ) Cl dT l dt

dT e = G el (T l (t) T e (t) ) + P(t) dt r r = G el (T e (t) T l (t) ) l T l (t,

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

1200

Temperature (K)

Laser pulse

1000 800 600 400 200

Telectrons TLattice
0 5 10 (ps) 15

IP

CM

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

Time

Phenomenological account for non-thermal effects


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)
I M PC S

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

Phenomenological approach to time dependent processes in metals 1)

(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)

M PC

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

2. Ultrafast laser optics of metals


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. .

M PC

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

Linear absorption spectrum of Cu nanoparticles

Optical density

0.8

Cu : 10 nm

0.4

0 1.8

Edp
2.2 2.6 (eV)

Edp : interband transition; quasi-particle/plasmon coupling

M PC

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

Pump-probe dynamics of Cu Nanoparticles


0

Delay (picoseconds)

1.2 0.8 0.4 0


1.8 2.0 2.2 2

Energy (eV)
J.-Y. Bigot, J.-C. Merle, O. Crgut, A. Daunois
M PC S

Phys. Rev. Lett., 75, 4702-4705 (1995).

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

Thermalization of electrons in metallic nanoparticles


F. Valle - Bordeaux

M PC

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

Surface plasmon dynamics


T/T (normalized)
1 ,0

Cu: 10 nm

2.255 eV 2.18 2.139

0 ,5

0 ,0 -1 0 1 2 3

Time delay (ps) Damping in nanoparticles : Kubos assumption

eff

= +

or + F g ( ) R

Origin of temperature dependent relaxation ?


I M PC S

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

Screened Coulomb potential in a metallic sphere


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

Many body calculation of damping associated to the Coulomb screening leads to :


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
M PC S

s ( ) 1

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

Femtosecond dynamics of Silver nanoparticles

Effect of the surface scattering on the linear response

Dynamical shift of the surface plasmon resonance

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

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

Dynamics of silver nanoparticles


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

0.20 0.15 0.10 0.05 0.00 -0.05 2.4 2.8 3.2

T / T normalized

0.75 0.50 0.25 0.00 -0.25

Te = 600 K 0.20 Te = 1200 K


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).
M PC S

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

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

M PC

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

3. The dynamics of magnetic metallic systems from femtomagnetism to the nanoscale


3.1 Ultrafast Magnetization Dynamics of thin ferromagnetic films
3.2 Ultrafast magnetization dynamics of nanostructures

M PC

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

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
I M PC S

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

Lattice Molecular vibrations, Phonons

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

1.0

M
0.5

C T Tc
Pierre Weiss

0.0

300

600

900

1200

Temperature (K)

TC

Time resolved spin thermometer


700 500 300 700 500 300

E(r,t)

probing Tspins with femtosecond temporal resolution


I M PC S

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

Time resolved ellipsometry


Kerr configuration: , reflection

Analyzers Faraday configuration:


, transmission

Pump pulse

t
Probe pulse: linear polarization

sample with magnetization M

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

and are measured for each pump-probe delay t M(t)


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

M PC

h
M

h
M

Ni thin films (M//) Phys. Rev. Lett. 76, 4250 (1996)

CoPt3 thin film (M) PRB, 58, 12134 (1998)


CoPt3 Kerr Signal (a.u.)

No pump

t =500 fs

-4

-2

0 2 H (kOe)

time
I M PC S

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

About light pulses interacting with spins

H S E(r,t)

e, p, V(r)

Dirac relatisvistic

ih

(r, t ) = c (p - eA(r, t )) + mc 2 + eV(r) (r, t ) t


Development in 1/c2

(central potential)

Spin orbit coupling

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

p4 eh eh 2 (p eA ) 2 H= .E p 2 2 divE + eV(r ) 2 2 2 2 2m 8m c 4m c 8m c eh i 2 2 .xE Dont forget me ! 8m c


I M PC S

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

Magnetization trajectory and Time domain Ferromagnetic Resonance


Heff
Co/Al2O3

M H0
Gilbert damping:

Pump :P(t)

Probe r dM dt r r r + M (t) Heff ( t ) = -P(t) M (t) r dM dt


damp

Femtosecond optical pulses

M PC

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

Ferromagnetic resonance induced with femtosecond optical pulses

600

Field ( Gauss )

16 nm Co/Al203 MBE grown

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

Time Delay ( ps ) 200 150 100 1 2 3 4

Period ( ps )

Applied field (kOe)


I M PC S

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

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

Ox : Pol = [S() S()] Oy : Long = [S() S()] Oz : Trans = [R() R()]

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

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

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

0 0 5 10 15 -2 20 0.0 0.2 0.4 0.6 0.8 1.0

Delay (ps)

Delay (ns)

M PC

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

Ultrafast Magnetization Dynamics visualized in 3D

16 nm Co/Al203
I M PC S

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

Precession dynamics in Co: perpendicular and parallel anisotropies

Co/Al2O3 HAnis sample


Pol/Pol x 10-2
0 -5 -10 -15
0 200 400 600

Co/MgO HAnis // sample


Pol/Pol x 10-2
4 0 -4

100

200

300

Delay (ps)

Delay (ps)

M PC

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

Model of time dependent magnetization dynamics with anisotropy


* 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

electrons lattice 0 time 20 ps

* Bloch equation or LL ( without assuming conservation of |M(t)| )


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

r r ~ r r H eff (t) = H 0 - N M(t) + H a (t)

* Temperature dependent magnetization modules


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

* Temperature dependent magneto-crystalline anisotropie r M(T )


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

M PC

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

In plane anisotropy

M PC

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

Beating of spin waves


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

Ipump = 0.97 mJ/cm-2 Ipump = 1.84 mJ/cm-2

0 order SW

Delay (ns)
Fourier Transform (a.u.) 1

T1 = 29.5 ps T0 = 35.9 ps T1 = 33.5 ps T0 = 45.6 ps


0 50 100

1st order SW

Frequency (GHz)
I M PC S

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

3. The dynamics of magnetic metallic systems from femtomagnetism to the nanoscale


3.1 Ultrafast Magnetization Dynamics of thin ferromagnetic films
3.2 Ultrafast magnetization dynamics of nanostructures

M PC

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

Dots with perpendicular magnetization Multi-domains structure


MFM imaging of CoPt3 dots
(d=1 m) (d=250 nm)

Some are mono-domains


I M PC S

Many are mono-domains

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

amplified Ti:S

(800 nm)

(400 nm)

Resolutions: spatial 300 nm, temporal 150 fs


I M PC S

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

Femtosecond magneto-optical confocal microscope


Magnet ( 0.4T)

H
PM F Analyzer F PM Scanning piezo
y x

Sample Focal plane Objective lens:

/2

Pinhole (20 m)

N.A = 0.65 (x 40)

.
R= 5x10- 4 R//
(400 nm) Polarization bridge

Dichroic Beam splitter

Polarizer

Probe (400 nm) Pump (800 nm)

5kHz amplified Ti:S Pulse duration ~120 fs

Optics letters 32, 936-398 (2007)


I M PC S

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

Individual 500 nm CoPt3 dot

Optics letters 32, 936-398 (2007)

Gauss250nm Crenel500nm

Gauss300nm Gauss900nm

Photo-induced dot on 15 nm film of CoPt3/Al2O3


I M PC S

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

Magnetization dynamics of single CoPt3 dot (1 m)


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

Pump fluence ( mJ cm-2 )

M PC

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

Dynamical imaging of a CoPt3 dot (1 m)

M PC

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

Laser induced writing-reading-erasing


-20 10 0 20

50

M (u.a)

-50x10

-6

Axe des X (m) 20 10 20 30 40 10

-10

Axe des X (m) 20 30 10

Axe des X (m) 20 30

15

M PC

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

Axe des Y (m) 10 15

Axe des Y (m)

Axe des Y (m)

10

15

10

Reading contrast with the MOPPI: CoPt3/Al2O3

Pump-probe delays
t = 300 fs t = 2 ps t = 10 fs

M PC

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

Writing a 150 nm single domain without external field CoPt/glass

Laser intensities : 4 mJcm-2 Pump 600 nm Kerr Images

8 mJcm-2

MFM Images

M PC

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

Magnetization dynamics of a single Permalloy dot (5 x 5 m2 on glass substrate)

0 P= 8 mJ cm-2 -0.5

Precession period = 230 ps

damping = 946 ps

M/M

-0.5

10 Delay (ps)

20

0.5 Delay (ns)

M PC

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

Dynamics of super-paramagnetic nanoparticles


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

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

Cobalt Nanoparticles Implanted in dielectric Matrices (glass, Al2O3)

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

-0.2 0 50 100 -1.5 -2 -1 0

Delay (ps)

1/p = 50 ps P = 90 ps

Long/Long (x10)

Phys. Rev. Lett. 97, 127401 (2006).


M PC S

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

Langevin approach : Brown 1963


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

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

For cobalt nanoparticles with diameter 4 nm in Al2O3:


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

0 = 55 ps !
2.5 nm = 3

The Gilbert damping varies with the size : = 2/MS0

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

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

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