Académique Documents
Professionnel Documents
Culture Documents
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Lycurgus Cup (Roman period : 4th century) exhibited at the British Museum.
Reflection
Transmission
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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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Ureter : 100 nm
70 mm
Courtesy : www.nanoprobes.com
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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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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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-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
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
ih
kl 1 k + q, l ' t
kl 1 k + q, l ' =
S
[ f o ( Ek + q ,l ' ) f o ( Ekl )]
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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
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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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 )
(a) (b)
2 r = 2 0 2 k d ( 2)
m d
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W=
sphere
S ds
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
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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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)
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Modify and study magnetization dynamics with light pulses Technology and fundamental physical processes
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-
elliptic non-rotated
k j
b ent ncid I eam
M
Re
fle cte d
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
(1)MO M i(1) () = ij () E j () j
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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
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
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
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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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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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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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)
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
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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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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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, )
( 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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athermal Distribution
(E)
(E)
EF
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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
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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Optical density
0.8
Cu : 10 nm
0.4
0 1.8
Edp
2.2 2.6 (eV)
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Delay (picoseconds)
Energy (eV)
J.-Y. Bigot, J.-C. Merle, O. Crgut, A. Daunois
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Cu: 10 nm
0 ,5
0 ,0 -1 0 1 2 3
eff
= +
or + F g ( ) R
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 / T normalized
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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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
E(r,t)
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
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h
M
h
M
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
(central potential)
eh 2 1 dV l.s 2 2 2m c r dr
M H0
Gilbert damping:
Pump :P(t)
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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 )
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
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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)
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16 nm Co/Al203
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100
200
300
Delay (ps)
Delay (ps)
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Temperature
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In plane anisotropy
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0 order SW
Delay (ns)
Fourier Transform (a.u.) 1
1st order SW
Frequency (GHz)
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amplified Ti:S
(800 nm)
(400 nm)
H
PM F Analyzer F PM Scanning piezo
y x
/2
Pinhole (20 m)
.
R= 5x10- 4 R//
(400 nm) Polarization bridge
Polarizer
Gauss250nm Crenel500nm
Gauss300nm Gauss900nm
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
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50
M (u.a)
-50x10
-6
-10
15
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10
15
10
Pump-probe delays
t = 300 fs t = 2 ps t = 10 fs
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8 mJcm-2
MFM Images
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0 P= 8 mJ cm-2 -0.5
damping = 946 ps
M/M
-0.5
10 Delay (ps)
20
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(a)
0.5
E / KV
Anisotropy K
dipolar
E
(b)
0.5
0 01
12 1
E / KV
00
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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)
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
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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
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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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