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Introduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 - Frontiers in Modern Optics, 30 June - 5 July, 2014. Robert W. Boyd University of Rochester University of Glasgow

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Page 1: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Introduction to Nonlinear Optics

University of Ottawa

P resented at the International School of Physics “Enrico Fermi,” Course 190 - Frontiers in Modern Optics, 30 June - 5 July, 2014.

Robert W. Boyd

University of RochesterUniversity of Glasgow

Page 2: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Outline of Presentation

Part I. Tutorial Introduction to Nonlinear Optics

Part II. Recent Research in Quantum Nonlinear Optics

Page 3: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 4: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Why Study Nonlinear Optics?

It is good fundamental physics.

It leads to important applications.

It is a lot of fun.

Demonstrate these features with examples in remainder of talk.

Page 5: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

1. What is Nonlinear Optics?

Page 6: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Nonlinear Optics and Light-by-Light Scattering

The elementary process of light-by-light scattering has never been observed in vacuum, but is readily observed using the nonlinear response of material systems.

M. A. Kramer, W. R. Tompkin, and R. W. Boyd, Phys. Rev. A, 34, 2026, 1986.W. R. Tompkin, M. S. Malcuit, and R. W. Boyd, Applied Optics 29, 3921, 1990.

Nonlinear material is fluorescein-doped boric acid glass (FBAG)n2 �)%$*��Ⱦ���14 n2(silica) [But very slow response!]

Page 7: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 8: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 9: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Fundamental Nonlinear Optical Processes: I

Second-Harmonic Generation

r (2)tt

2t

t

t

2t

Dolgaleva, Lepeshkin,and Boyd

Page 10: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Fundamental Nonlinear Optical Processes: II

Sum-Frequency Generation

r (2)

t1

t 2

t1

t 2

t3

t3 = t1 +t2

Page 11: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Fundamental Nonlinear Optical Processes: III

Difference-Frequency Generation

r (2)t

2t

1

t2

t3

t1 t

3= t

1< t

2

Optical Parametric Oscillation

amplified!

Page 12: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Parametric Downconversion: A Source of Entangled Photons

The signal and idler photons are entangled in:

(a) polarization

(b) time and energy

(c) position and transverse momentum

(d) angular position and orbital angular momentum

t

t

t

Entanglement is important for:(a) Fundamental tests of QM (e.g., nonlocality) (a) Quantum technologies (e.g., secure communications)

Page 13: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Fundamental Nonlinear Optical Processes: III

Third-Harmonic Generation

tt

t

t

3t3tr (3) t

Page 14: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Fundamental Nonlinear Optical Processes: IV

Intensity-Dependent Index of Refraction

r (3)

r (3)

E(t )

E(t )

E(t ' ) E(t ' ) eiqNL

E(t ) eiqNL

(strong wave)

(probe wave)

��6LQJOH�EHDP� self-phase modulation

��7ZR�EHDP� cross-phase modulation

7KH�UHIUDFWLYH�LQGH[�LV�JLYHQ�E\

where

Page 15: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Role of Material Symmetry in Nonlinear Optics

x

U(x)

parabolaactual

potential

parabola

x

U(x)

parabola

actual potential

parabola

centrosymmetric medium

non-centrosymmetric medium

r(2) vanishes identically for a material possessing a center of inversion sym- metry (a centrosymmetric medium).

Page 16: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

2. Coupled Wave Equations and HarmonicGeneration

Page 17: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Treatment of Second-Harmonic Generation – I

ω 2ω

L

z

χ (2)E1, E2,

LetE1(z, t) = E1(z)e

�i!t + c.c. = A1ei(k1z�!t) + c.c. (1)

E2(z, t) = E2(z)e�i2!t + c.c. = A2(z)e

i(k2z�2!t) + c.c. (2)

where k1 = n1!/c and k2 = n22!/c.

We have assumed that the pump wave E1 at frequency ! is unde-pleted by the nonlinear interaction. We take A2 to be a function of zto allow the second harmonic wave to grow with z. We also set

P2(t) = P2 e�i2!t where P2 = ✏0�

(2)E21 = ✏0�

(2)A21 e

i2k1z (3)

The generation of the wave at 2! is governed by the wave equation

r2E2 �n2

c2@2E2

@t2=

1

✏0c2@2P2@t2

. (4)

Page 18: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Treatment of Second-Harmonic Generation – II

Note that the first term in the wave equation is given by

r2E2 =

2

666664

@2A2

@z2+ 2ik2

@A2

@z� k22A2

3

777775ei(k2z�2!t) (5)

⇡2

6666642ik2

@A2

@z� k22A2

3

777775ei(k2z�2!t) (6)

The second form is the slowly varying amplitude approximation.

Note also that@2A2

@t2= �(2!)2A2 e

i(k2z�2!t) @2P2@t2

= �(2!)2P2 ei(2k1z�2!t) (7)

By combining the above equations, we obtain

2ik2dA2

dz=

�4!2

c2�(2)A2

1ei�k z where �k = 2k1 � k2. (8)

The quantity �k is known as the phase (or wavevector) mismatchfactor, and it is crucially important in determining the e�ciency ofnonlinear optical interactions

Page 19: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Treatment of Second-Harmonic Generation – III

For the case �k = 0, Eq. (8) becomes

2ik2dA2

dz=

�4!2

c2�(2)A2

1 (9)

with solution evaluated at z = L of

A2(L) =2i!

n2c�(2)A2

1L or |A2(L)|2 =4!2

n22c2[�

(2)]2|A1|4L2. (10)

Note that the SHG intensity scales as the square of the input intensityand also as the square of the length L of the crystal.

ω2

ω2

dipole emitter phased array of dipoles

Page 20: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Treatment of Second-Harmonic Generation – IV

For the general case of �k 6= 0, Eq. (8) can still be solved to yield

|A2(L)|2 =4!2

n22c2 [�(2)]2 |A1|4L2 sinc2(�k L/2) (11)

Note that �k L must be kept much smaller than ⇡ radians in orderfor e�cient SHG to occur.

Page 21: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Second Harmonic Generation and Nonlinear Microscopy

Nonlinear Optical Microscopy

An important application of harmonic generation is nonlinear microscopy. . .

Microscopy based on second-harmonic generation in the configuration of a confocal microscope and excited by femtosecond laser pulses was introduced by Curley et al. (1992). Also, harmonic-generation microscopy can be used to form images of transpar-ent (phase) objects, because the phase matching condition of nonlinear optics depends sensitively on the refractive index variation within the sample being imaged (Muller et al., 1998).

Boyd, NLO, Subsection 2.7.1

RWB
Page 22: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Caution!

Curley et al., not Curly et al.

Page 23: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

How to Achieve Phase Matching: Birefringence Phase Matching

The phase matching condition �k = 0 requires thatn1!1

c

+n2!2

c

=n3!1

c

where !1 + !2 = !3

These conditions are incompatible in an isotropic dispersive material.However, for a birefringent material phase matching can be achieved.

ω 2ωθ kc

ordinary extraordinary

Midwinter and Warner showed that there are two ways to achieve phase matching:

Positive uniaxial Negative uniaxial(n

e

> n0) (ne

< n0)

Type I n

03!3 = n

e

1!1 + n

e

2!2 n

e

3!3 = n

o

1!1 + n

o

2!2

Type II n

03!3 = n

o

1!1 + n

e

2!2 n

e

3!3 = n

e

1!1 + n

o

2!2

Page 24: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

How to Achieve Phase Matching: Quasi Phase Matching

Λ

single domain crystal periodically poled crystal

Sign of �(2) is periodically inverted to prevent reverse power flow.

0 2 4 6 8

z / Lcoh

fiel

d am

plitu

de

0

(a) with perfect phase-matching

(c) with a wavevector mismatch

(b) with quasi-phase-matching

Page 25: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 26: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Additional Studies of Wave Propagation Effects

Page 27: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

3. Mechanisms of Optical Nonlinearity

Page 28: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Typical Values of the Nonlinear Refractive Index

n2a �(3)

1111 Response timeMechanism (cm2/W) (m2/V2) (sec)

Electronic polarization 10�16 10�22 10�15

Molecular orientation 10�14 10�20 10�12

Electrostriction 10�14 10�20 10�9

Saturated atomic absorption 10�10 10�16 10�8

Thermal e↵ects 10�6 10�12 10�3

Photorefractive e↵ectb (large) (large) (intensity-dependent)

a For linearly polarized light.b The photorefractive e↵ect often leads to a very strong nonlinear response. This response usually

cannot be described in terms of a �(3) (or an n2) nonlinear susceptibility, because the nonlinear po-

larization does not depend on the applied field strength in the same manner as the other mechanisms

listed.

Page 29: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

,,

ω p

ω q

(a1 )

ω p

ω q

(a 2 )

ω p

ω q ω p

ω q

(a'1a'2 )

ω p

ω q ω p

ω q

ω p

ω q ω p

ω q

(b1)

b'1

b'2 )

l l

n

m

ll

l l

n

m

l l

n n

m

l l

n n

m

l l

n n

m

l l

n n

m

l l

m m

n

ll

m m

n

l l

) (

Quantum Mechanical Origin of the Nonlinear Optical Suesceptibility

(b )2

Page 30: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 31: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 32: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 33: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Some Actual Z-Scan Data

M. Sheik-Bahae et al., IEEE J. Quantum Electron. 26 760 (1990).

1.0

z (mm)

1.2

0.820–20 0

n2 = 0.0373 cm2/GW

I0 = 0.176 GW/cm2

CS2

Closed aperture Open aperture

gold-silica composite

z (mm)

0.9

1.0

1.1

1.2

–125 125 0

Piredda

Chang, Shin

tran

smis

sion

tran

smis

sion

ΔTpv = 0.406 ΦNL

For closed aperture z-scan

ΦNL = n2 (ω/c) Ι0 Lwhere

Page 34: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

6. Self-Action Effects in Nonlinear Optics

Page 35: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Self-Action Effects in Nonlinear Optics

Self-action effects: light beam modifies its own propagation

d

Page 36: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 37: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Prediction of Self Trapping

de

ve

n = n0

n = n0

n = n0 +bn

radial profile of self-trapped beam

Page 38: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 39: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Optical Solitons

Field distributions that propagate without change of form

Temporal solitons (nonlinearity balances gvd)

Spatial solitons (nonlinearity balances diffraction)

1973: Hasegawa & Tappert1980: Mollenauer, Stolen, Gordon

1964: Garmire, Chiao, Townes1974: Ashkin and Bjorkholm (Na)1985: Barthelemy, Froehly (CS2)1991: Aitchison et al. (planar glass waveguide1992: Segev, (photorefractive)

Page 40: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Solitons and self-focussing in Ti:Sapphire

Diffraction-management controls the spatial self-focussing

Dispersion-management controls the temporal self-focussing

Page 41: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Beam Breakup by Small-Scale Filamentation

Predicted by Bespalov and Talanov (1966)

Exponential growth of wavefront imperfections by four-wave mixing processes

transverse wavevector, q/qmax

expo

nent

ial g

row

th ra

te,�R

/a

Sidemode amplitude grows as A1(z) = A1(0)eiazeRz

a = n2 (t / c)I0,

R2 =q2

2k2a <

q2

2k

£

¤ ² ²

¥

¦ ´ ´ ,

q = k�

qmax = 2ka

emax =qmaxk

Page 42: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Honeycomb Pattern Formation

Output from cell with a single gaussian input beam

Quantum statistics?

Input power 100 to150 mWInput beam diameter 0.22 mm

Sodium vapor cell T = 220o CWavelength = 588 nmBennink et al., PRL 88, 113901 2002.

At medium input power At high input power

at cell exit in far field at cell exit in far field

Page 43: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

n2 mediumspatiallycoherent light in

spatially incoherentlight out

Incident pulse enerJ\��ȝ-�1000

0.4

0.8

1.2

1.6

Far-f

ield

difIUDFWLRQ�DQJOH��GHJ�

Optical Radiance Limiter Based on Spatial Coherence Control

Controlled small-scale filamentation used to modify spatial degree of coherence

Alternative to standard appropches to optical power limiting

Schweinsberg et al., Phys. Rev. A 84, 053837 (2011). 20 30

increasing power

Page 44: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

4. Local-Field Effects in Nonlinear Optics

Page 45: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Local Field Effects in Nonlinear Optics – I

Recall the Lorentz-Lorenz Law(linear optics)

χ(1) =Nα

1 − 43πNα

orϵ(1) − 1

ϵ(1) + 2=

4

3πNα.

E PEloc

This result follows from the assumption that the field that acts on arepresentative atom is not the macroscopic Maxwell field but ratherthe Lorentz local field given by

Eloc = E + 43πP where P = χ(1)E

We can rewrite this result as

Eloc = LE where L =ϵ(1) + 2

3is the local field factor.

Page 46: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

See, for instance, H. A. Lorentz, Theory of Electrons, Dover, NY (1952).

The Lorentz Red Shift

Page 47: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Maki, Malcuit, Sipe, and Boyd, Phys. Rev. Lett. 68, 972 (1991).

Observation of the Lorentz Red Shift

Page 48: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Local Field Effects in Nonlinear Optics – II

For the case of nonlinear optics, Bloembergen (1962, 1965) showedthat, for instance,

χ(3)(ω = ω + ω − ω) = Nγ(3)|L(ω)|2[L(ω)]2.

where γ(3) is the second hyperpolarizability and where

L(ω) =ϵ(ω) + 2

3

For the typical value n = 2, L = 2, and L4 = 16. Local field effectscan be very large in nonlinear optics! But can we tailor them for ourbenefit?

We have been developing new photonic materials with enhanced NLOresponse by using composite structures that exploit local field effects.

Page 49: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Nanocomposite Materials for Nonlinear Optics��0D[ZHOO�*DUQHWW ��%UXJJHPDQ���LQWHUGLVSHUVHG)

� Fractal StrXFWXUe ��LayerHGh

2a

b

¡i

¡h

¡a¡b

¡a

¡b

- In each case, scale size of inhomoJeneity << optical ZaveleQJWK

-�7KXs all optical properties, VXch as n anG Ƶ���, can be�GescribeG by effective �YROXPH�DYHrDJHG)�YDOXHs

5HFHQW�UHYLHZ��'ROJDOHYD�DQG�%R\G��$GYDQFHV�LQ�2SWLFV�DQG�3KRWRQLFV�����²�����������

Page 50: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Local Field Enhancement of the NLO Response- Under very general conditions, we can express the NL

response as eff(3) = f L2 L 2 (3)

L = + 23

- For a homogeneous material

L = 3 h

m + 2 h

For a spherical particle of dielectric constant embedded in a host of dielectic constant

m

h

where f is the volume fraction of nonlinear material and L is the local-field factor, which is different for each material geometry.

- Under appropriate conditions, the product can exceed unity. f L2 L 2

-

For a layered geometry with the electric field perpendicular to theof the layers, the local field factor for component a is given by

L = eff

a

1eff

=fa

a

+fb

b

-

plane

Page 51: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Alternating layers of TiO2 and the conjugated polymer PBZT.

Fischer, Boyd, Gehr, Jenekhe, Osaheni, Sipe, and Weller-Brophy, Phys. Rev. Lett. 74, 1871 (1995).

Measure NL phase shift as a function of angle of incidence.

A composite material can display a larger NL response than its constituents!

Enhanced NLO Response from Layered Composite Materials

3.2 times enhancement!35% enhancement in r(3)

Diode Laser(1.37 um)

polarizer

photodiode

gold electrode

ITO

BaTiO3

1 kHz

lockin amplifier

signal generator

dc voltmeter

glass substrate

AF-30 inpolycarbonate

Quadratic EO effect

Nelson and Boyd, APL 74 2417 (1999)

Page 52: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

E

z

Cu

L0

E

z

Cu

� Metals have very large optical nonlinearities but low transmission

� Solution: construct metal-dielectric photonic crystal structure(linear properties studied earlier by Bloemer and Scalora)

80 nm of copperT = 0.3%

� Low transmission because metals are highly reflecting (not because they are absorbing!)

Accessing the Optical Nonlinearity of Metals with Metal-Dielectric Photonic Crystal Structures

SiO2 PC structure

bulk metal 80 nm of copper (total)

T = 10%

h�������nm

I = 500 MW/cm2

M/D PC

bulk Cu

(response twelve-times larger)

Bennink, Yoon, Boyd, and Sipe, Opt. Lett. 24, 1416 (1999).

Lepeshkin, Schweinsverg, Piredda, Bennink, and Boyd, Phys. Rev. Lett. 93, 123902 (2004).

Page 53: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 54: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

Gold-Doped Glass: A Maxwell-Garnett Composite

gold volume fraction approximately 10-6

gold particles approximately 10 nm diameter

• Red color is because the material absorbs very strong in the blue, at the surface plasmon frequency

• Composite materials can possess properties very differentfrom those of their constituents.

Developmental Glass, Corning Inc.

Red Glass CaraffeNurenberg, ca. 1700

Huelsmann Museum, Bielefeld

Page 55: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -
Page 56: Introduction to Nonlinear Optics · PDF fileIntroduction to Nonlinear Optics University of Ottawa P resented at the International School of Physics “Enrico Fermi,” Course 190 -

8

6

9

4

1

7

2

5

3

-10 0 10 20 30z (cm)

0.5

0.6

0.7

0.8

0.9

1.0

1.1

1.2

1.3

D.D. Smith, G. Fischer, R.W. Boyd, D.A.Gregory, JOSA B 14, 1625, 1997.

Increasing Gold

Content

2(3) (3) (3)eff i h

f L= +L2

norm

aliz

ed tr

ansm

ittan

ce

Counterintuitive Consequence of Local Field Effects

Cancellation of two contributions that have the same signGold nanoparticles in a reverse saturable absorber dye solution (13 μM HITCI)

(3)Im < 0

(3)Im > 0

RSA

SAβ < 0

β > 0

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Is there an intrinsic nonlinear reponse to surface plasmon polaritons (SPPs)?��$�QRQOLQDU�UHVSRQVH�ZRXOG�EH�XVHIXO�IRU�SKRWRQLFV�DSSOLFDWLRQV��0HWDOV�DUH�KLJKO\�QRQOLQHDU��Q2 is106 times that of silica)��+LJK��VXE�ZDYHOHQJWK��ILHOG�FRQILQHPHQW�LQ�DQ�633

NLO in Plasmonics (Photonics Using Metals)

���%XW�633V�WHQG�WR�VKRZ�KLJK�ORVV

SRZHU�YDULHV�IURP���WR����P:���LQWHQVLW\�YDULHV�IURP���WR����*:�FP

0HDVXUH�LQWHQVLW\�GHSHQGHQFH�RI�WKH�.UHWVFKPDQQ�DQJOH

Au film

Laser

Translation stage

Rotation stage

HWP PBSPD

TMpolarized

Aperture

x z

y

Refle

ctan

ce, R

1.0

0.5

0.05

0.1

TIR onset

Kretschmann dip

increasingpower Pi = 2.70 mW

Pi = 8.70 mWPi = 15.0 mWPi = 22.8 mWPi = 28.4 mW

41.5 42 42.5 43 43.5Incidence angle, (deg.)

Ȗsp ������î�����:��

Ȗsp� ������î�����:��

ț sp����

6 ��UDG�P�

ț sp����

� ����P�

633�SHDN�SRZHU�GHQVLW\� Ssp ��*:�P�

������

������

������

������

����������

����

����

����

����

0 1 2 3 ���ƍ

ƍƍƍ

Ǝ

ODVHU�ZDYHOHQJWK�LV�������QPODVHU�SXOVH�GXUDWLRQ�LV�����IV

I. De Leon, Z. Shi, A. Liapis and R.W.Boyd, Optics Letters 39, 2274 (2014)

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Slow Light in a Fiber Bragg Grating (FBG) Structure(Can describe properties of FBGs by means of analytic expressions)

t

kJ

tJ

k

slow light

dispersion relationforward and backward wavesare strongly coupled

theory (Winful)

detuning from Bragg frequencystore

d en

ergy

(sam

e as

gro

up in

dex) KL = 4

��(QKDQFHG�1/2�UHVSRQVH�

where the slow-down factor S = ng/n

Bhat and Sipe showed that the nonlinear coeficient is given by

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group index approximately 140

Improved Slow-Light Fiber Bragg Grating (FBG) StructureMuch larger slow-down factors possible with a Gaussian-profile grating

H. Wen, M. Terrel, S. Fan and M. Digonnet, IEEE Sensors J. 12, 156-163 (2012).

Observation of (thermal)optical bistability at mWpower levels

J. Upham, I. De Leon, D. Grobnic, E. Ma, M.-C. N. Dicaire, S.A. Schulz, S. Murugkar, and R.W. Boyd, Optics Letters 39, 849-852 (2014).

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The other Lake Como

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5. Slow and Fast Light

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Controlling the Velocity of Light

– Light can be made to go: slow: vg << c (as much as 106 times slower!) fast: vg > c backwards: vg negative Here vg is the group velocity: vg = c/ng ng = n + Ʒ (dn/dƷ)

Review article: Boyd and GautKier, Science 326, 1074 (2009).

“Slow,” “Fast” and “Backwards” Light

– Velocity controlled by structural or material resonancesabsorption

profile

RWB
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n

ng

t

t

t

t 0

absorptionresonance

slow light

fast light

_

n

ng

t

t

t

t 0

gainresonance

g

fast light

slow light

Slow and Fast Light Using Isolated Gain or Absorption Resonances

ng = n + Ʒ (dn/dƷ)

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Light speed reductionto 17 metres per secondin an ultracold atomic gasLene Vestergaard Hau*², S. E. Harris³, Zachary Dutton*²& Cyrus H. Behroozi*§

NATURE | VOL 397 | 18 FEBRUARY 1999 |www.nature.com

1.8 GHz

60 MHz

D line

λ = 589 nm

ω ωc p

|2 = |F =2, M = –2〉 〉F

|1 = |F =1, M = –1〉 〉F

|4 = |F =3, M = –2〉 〉F

|3 = |F =2, M = –2〉 〉F

2

–30 –20 –10 0 10 20 30

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

Tra

nsm

issio

n

a

–30 –20 –10 0 10 20 30

Probe detuning (MHz)

0.994

0.996

0.998

1.000

1.002

1.004

1.006

Refr

active index

b

–2 0 2 4 6 8 10 12

Time (μs)

0

5

10

15

20

25

30

PM

T s

ign

al (m

V)

T = 450 nK

τDelay

= 7.05 ± 0.05 μs

L = 229 ± 3 μm

vg = 32.5 ± 0.5 m s

–1

* Rowland Institute for Science, 100 Edwin H. Land Boulevard, Cambridge,Massachusetts 02142, USA² Department of Physics, § Division of Engineering and Applied Sciences,Harvard University, Cambridge, Massachusetts 02138, USA³ Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305, USA

Note also related work by Chu, Wong, Welch, Scully, Budker, Ketterle, and many others

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Crucial for many real-world applications

We have identified two preferred methods for producing slow light

(1) Slow light via coherent population oscillations (CPO)

(2) Slow light via stimulated Brillouin scattering (SBS)

Goal: Slow Light in a Room-Temperature

Solid-State Material

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Slow Light by Stimulated Brillouin Scattering (SBS)

1t

L

tS

dI Sdz

= ïgILIS

g = Ƣ2eƷ2

nv c3Ư0ƊB.

z

We often think of SBS as a pure gain process, but it also leads to a change in refractive index

t�� t - 1S L

SBS

gain

refra

ctiv

e in

dex

monochromatic pump laser

Stokes gain

anti-Stokes loss

slow light fast light

Ʒ

Ʒ

TdG

BThe induced time delay is where G= g Ip L and is the Brillouin linewidth B

=

Okawachi, Bigelow, Sharping, Zhu, Schweinsberg, Gauthier, Boyd, and Gaeta Phys. Rev. Lett. 94, 153902 (2005). Related results reported by Song, González Herráez and Thévenaz, Optics Express 13, 83 (2005).

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Slow Light via Coherent Population Oscillations

PRL 90,113903(2003); Science, 301, 200 (2003)

� Ground state population oscillates at beat frequency b (for b < 1/T1).

Kba=

1T

12a

ba=

2T

2

a

bsaturablemedium

t

t + b t + b

E1,

E3,

measureabsorption

� Population oscillations lead to decreased probe absorption (by explicit calculation), even though broadening is homogeneous. � Ultra-slow light (ng > 106) observed in ruby and ultra-fast light (ng = –4 x 105) observed in alexandrite.

� Slow and fast light effects occur at room temperature!

absorptionprofile

Want a narrow feature in absorption profile to give a large dn/dt�

ng = n + t�dn/dt��� 1/T1

1/T2

T2 << T1

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Slow and Fast Light in an Erbium Doped Fiber Amplifier

6 ms

outin

• Fiber geometry allows long propagation length• Saturable gain or loss possible depending on pump intensity

-0.1

-0.05

0

0.05

0.1

0.15

Frac

tiona

l Adv

ance

men

t

10 100Modulation Frequency (Hz)

10 3 10 4 10 5

- 97.5 mW- 49.0 mW- 24.5 mW- 9.0 mW- 6.0 mW- 0 mW

Advance = 0.32 ms

InputOutput

Time

FWHM = 1.8 ms

Schweinsberg, Lepeshkin, Bigelow, Boyd, and Jarabo, Europhysics Letters, 73, 218 (2006).

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Observation of Backward Pulse Propagation in an Erbium-Doped-Fiber Optical Amplifier

0 2 4 6

0

1

2

3

time (ms)

norm

aliz

ed in

tens

ity

in

out

We time-resolve the propagation of the pulse as a function of position along the erbium-doped fiber.Procedure • cutback method • couplers embedded in fiber

1550 nm laser ISO80/20

coupler

980 nm laserWDM

WDM1550980

EDF

Ref

Signal

or

G. M. Gehring, A. Schweinsberg, C. Barsi, N. Kostinski, R. W. Boyd, Science 312, 985 2006.

pulse is placed on a cw background to minimizepulse distortion

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Observation of Superluminal and

“Backwards” Pulse Propagation

rcoun erin v

B n rc en

y

Normalized length |ng|Z (m)0 0.5-0.5 1x10-1 5

6t = 0

6t = 3

6t = 6

6t = 9

6t = 12

6t = 15

or or rconc r c

G ring,

c ,

propagation distance

ng negative

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time

puls

e am

plitu

de

road spectral content at points of discontinuityce moves at vacuum speed of light

see, for instance, R. Y. Chiao

Causality?

g g

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8. Spontaneous and Stimulated Light Scattering

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Experiment in Self Assembly

Joe Davis, MIT

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Thank you for your attention!