Ultrafast Optics

Definition: the generation, measurement, and application of

ultrashort laser pulses

The birth and history of ultrafast optics

Measuring ultrashort pulses Prof. Rick Trebino

Georgia Tech
Shaping ultrashort pulses www.frog.gatech.edu

Ultrafast spectroscopy

Medical imaging
The Birth of Ultrafast Technology

Bet: Do all four

hooves of a
galloping horse ever
simultaneously leave
the ground?
Leland Stanford Eadweard Muybridge

Palo Alto, CA 1872

Time Resolution:
1/60th of a second
Harold Edgerton: Strobe Photography
How to Make
Apple sauce
at MIT
1964

Harold
Edgerton
MIT, 1942

Splash on a
Glass
Curtis Hurley
Junior High
School
student
1996

Time resolution: a few microseconds

Pulsed Pumping: s Pulses

Pumping a laser medium with a short-pulse flash lamp yields a

fairly short pulse. Flash lamp pulses as short as ~1 s exist.

Unfortunately, this yields a pulse as long as the excited-state

lifetime of the laser medium, which can be considerably longer
than the pump pulse.

Since solid-state laser media have lifetimes in the microsecond

range, it yields pulses microseconds to milliseconds long.

I(t)

Long and potentially

complex pulse
Q-Switching: ns Pulses

Q-switching involves: Output pulse intensity

Preventing the Gain

laser from lasing saturation
(by adding 100%

Cavity Gain
Cavity Loss
massive loss)
until the flash
lamp is finished
flashing, and
0%
Abruptly allowing Time
the laser to lase.

The pulse length is limited by how fast we can switch and the
round-trip time of the laser and yields pulses 10 - 100 ns long.
Ultrafast optics vs. electronics
6
Timescale (seconds) 10

9
10
Electronics

12
10

Optics
15
10

1960 1970 1980 1990 2000

Year

No one expects electronics to ever catch up.

The metric system
Well need to really know the metric system because the pulses are
incredibly short and the powers and intensities can be incredibly high.

Prefixes:

Small Big

milli (m) 10-3 Kilo (k) 10+3

micro () 10-6 Mega (M) 10+6
nano (n) 10-9 Giga (G) 10+9
pico (p) 10-12 Tera (T) 10+12
femto (f) 10-15 Peta (P) 10+15
atto (a) 10-18 Exa (E) 10+18
 Timescales
Its routine to generate pulses < 1 picosecond (10-12 s) long.
Researchers generate pulses a few femtoseconds (10 -15 s) long.

Computer Camera One Age of Human existence

10 fs light clock cycle flash month pyramids
pulse 1 minute Age of universe

10-15 10-12 10-9 10-6 10-3 100 103 106 109 1012 1015 1018
Time (seconds)
1 femtosecond 1 picosecond

Such a pulse is to a minute as a minute is to the age of the universe.

Such a pulse is to a second as 5 cents is to the US national debt.

The Ti:Sapphire Laser, Including
Dispersion Compensation
Adding two prisms compensates for GDD in the Ti:Sapphire crystal
and mirrors.

Ti:Sapphire Slit for

cw pump beam
gain medium tuning

Prism dispersion
compensator

This is currently the workhorse laser of the ultrafast optics community.

Typical properties: 800 nm wavelength, 100 fs pulse length, 1 nJ
pulse energy, 100 MHz rep rate
Ultrafast set-ups can be very sophisticated.
Unbelievably High iIntensities!

National Ignition
Facility (under
construction)
192 shaped pulses
>1 MJ total energy
~ 10 Petawatts
The vast majority of humankinds greatest
discoveries have resulted directly from
improved techniques for measuring light.
Microscopes led to biology.

Telescopes led X-ray crystallography

to astronomy. solved DNA.

Spectrometers led to quantum mechanics.

l

The Michelson interferometer led to relativity.

And technologies, from medical imaging to

GPS, result from light measurement!
Frontiers of Light Measurement: Ultrafast
and Complex
Most light is broadband and hence ultrafastwith temporal structure
as short as the shortest events ever created.
Complex pulse

Complex in time
Intensity

Phase
Ultrabroadband supercontinuum
Arbitrary waveforms
Time

Complex in time and space

Nearly every pulse near a focus
Focusing pulse seen
Pulses emerging from almost any medium from the side
The Dilemma

In order to measure
an event in time,
you need a shorter one.

To study this event, you need a

strobe light pulse thats shorter.
Photograph taken by Harold Edgerton, MIT

But then, to measure the strobe light pulse,

you need a detector whose response time is even shorter.

And so on

So, now, how do you measure the shortest event?

A laser pulse has an intensity and phase
vs. time or frequency.
Its electric field can be written:

{ }

Intensity, I(t)
I (t ) exp [ i (w0t - f (t )) ]

Phase, f(t)
E (t ) Re
Intensity Phase
Time

Alternatively, in the frequency domain:

Spectrum, S(w)
(w ) S (w ) exp [ -ij (w ) ]
E%

phase, j(w)
Spectral
Spectrum Spectral
Phase Frequency

We need to measure both the temporal (or spectral) intensity and

phase.
One-Dimensional Phase Retrieval
Its more interesting than it appears

Spectrum, S(w)

phase, j(w)
to ask what we lack when we know

Spectral
only the pulse spectrum S(w ).

Recall: (w ) S (w ) exp [ -ij (w )]

E% Frequency

Obviously, what we lack is the spectral phase j (w ).

time

Retrieving it is called the 1D phase retrieval problem.

Even with extra information,

its impossible.
E.J. Akutowicz, Trans. Am. Math. Soc. 83, 179 (1956)
E.J. Akutowicz, Trans. Am. Math. Soc. 84, 234 (1957)
Pulse Measurement in the time domain:
The Intensity Autocorrelator
Crossing beams in a nonlinear-optical crystal, varying the
delay between them, and measuring the signal pulse energy
vs. delay, yields the Intensity Autocorrelation, A(2)().
Pulse to
be
measure
d The signal field is E(t) E(t- ).
Beam So the signal intensity is I(t) I(t- )
SHG
splitter crystal
E(t)
SHG
crystal Detector

Esig(t,)
Variabl E(t)
e
delay,
The Intensity A(2) ( )
I (t ) I ( t - ) dt
Autocorrelation:
-
Pulses and Their Autocorrelations
Pulse Intensity Autocorrelation

Gaussian
1.41x
shape:
wider

Time Delay

sech2
1.54x
shape:
wider

Time Delay

Since a theoretical model of one ultrafast laser predicts a sech 2 pulse

shape, everyone always divides the autocorrelation width by 1.54 and
calls it the pulse width. Even when the autocorrelation is Gaussian
 Autocorrelation of a Complex Pulse
As the pulse Intensity Autocorrelation
intensity increases
in complexity, its
autocorrelation
approaches a
background plus a
narrow coherent
artifact.

Retrieving the
intensity from Coherent
artifact
the
autocorrelation
is fundamentally
impossible!
Retrieving the intensity from its autocorrelation is also equivalent to the
one-dimensional phase-retrieval problem!
The Spectrogram of a Waveform E(t)
Its the spectrum of the product E(t) g(t-) for all delays, .

Example: E (t )
Linearly
Light electric field

chirped
Gaussian g(t-) gates
pulse out a piece
of E(t),
centered
at .

g(t-)
0 Time (t)

The spectrogram yields the color and intensity of E(t) at the time, .
Spectrograms for Linearly Chirped Pulses

Negatively chirped Unchirped Positively chirped

Frequency

Time
Frequency

Delay

Like a musical score, the spectrogram visually displays the frequency

vs. time (and the intensity, too).
Properties of the Spectrogram
Algorithms exist to retrieve E(t) from its spectrogram.
The spectrogram essentially uniquely determines the waveform intensity,
I(t), and phase, f (t) [and, equivalently, S(w ) and j (w )].

The gate need not beand should not bemuch shorter than E(t).
Suppose we use a zero-width gate pulse:
It would gate out an infinitely short chunk of the pulse, which
would have an infinitely broad spectrumproviding no color
(phase) information at all!

The spectrogram resolves the dilemma! It doesnt need the shorter

event! It temporally resolves the slow components and spectrally
resolves the fast components.
Spectrogram pulse retrieval is equivalent to the 2D Phase Retrieval
Problema well-behaved problem, which works because the
Fundamental Theorem of Algebra fails for polynomials of two variables!
Frequency-Resolved Optical Gating
(FROG)
FROG is simply a spectrally resolved
Pulse to be autocorrelation, which is a spectrogram.
measured

Beam I FROG (w , ) = Spectrum

Esig (t , )

splitter

E(t) Camera
SHG
crystal Spec-
trometer

Variable E(t) Esig(t,)= E(t) E(t-)

delay,

FROG can use any fast nonlinear-optical process.

SHG FROG is the most sensitive version.
One of the Shortest Events Ever Created!

FROG traces

A 4.5 fs pulse!

Baltuska,
Pshenichnikov,
and Weirsma,
J. Quant. Electron.,
35, 459 (1999).
FROG measurement of ultrabroadband
continuum
Retrieved intensity
Ultrabroadband continuum was created and phase
by propagating 1-nJ, 800-nm, 30-fs
pulses through 16 cm of microstructure
fiber.
Spectrogram

This pulse has a time-bandwidth product

of ~ 4000, and is the most complex
ultrashort pulse ever measured.
For a fully narrated talk on how to
measure ultrashort pulses, go to
www.frog.gatech.edu, click on
Talks, and click this icon:
Phase Wrapping and Unwrapping
Technically, the phase ranges from to . But it often helps to make
it a continuous function, that is, to unwrap it. This involves adding or
subtracting 2 whenever theres a 2 phase jump.

Example: a pulse with quadratic phase Note the scales!

Wrapped phase Unwrapped phase

Time or frequency Time or frequency

The main reason for unwrapping the phase is aesthetics.

But it often helps us discern the shape of the phase.
Phase-Blanking
When the intensity is zero, the phase is meaningless (whats the
color of darkness?).
When the intensity is nearly zero, the phase is nearly meaningless.
Phase-blanking involves simply not plotting the phase when the
intensity is close to zero.

Without phase blanking With phase blanking

Time or frequency Time or frequency

The only problem with phase-blanking is that you have to decide the
intensity level below which the phase is meaningless.
Beam Propagation
What happens to a pulse as it propagates through a medium?
Always model (linear) propagation in the frequency domain. Also,
you must know the entire field (i.e., the intensity and phase) to do so.

Ein (t ) Eout (t )
t a (w ) t
n(w )
E%in (w ) E%out (w )
w w

E%
out (w ) = %(w ) exp[-a (w ) L / 2] exp[-in(w )kL]
Ein

In the time domain, propagation is a convolutionmuch harder.

How do we shape a pulse?
We could try to modulate the pulse directly in time.

Eout ( t ) = h ( t ) Ein ( t )

Unfortunately, this requires a very fast modulator, and existing

modulators are too slow.

Alternatively, we can modulate the spectrum.

out ( w ) = H ( w ) Ein ( w )
E% %

So all we have to do is to frequency-disperse the pulse in space

and modulate the spectrum and spectral phase by creating a
spatially varying transmission and phase delay.
The Pulse
Shaper
x l(x)

grating grating
f f
f f
f f
Recall that this geometry maps angle (and
hence wavelength) to position at this plane,
called the Fourier transform plane!

How it works:
The grating disperses the light, mapping color onto angle.
The first lens maps angle (hence wavelength) to position.
The second lens and grating puts the pulse back together.

The trick is to place a mask in the l(x) plane.

A phase mask selectively delays colors.

An amplitude mask shapes the spectrum.

The Pulse-
Shaper
Amplitude mask Phase mask
Transmission = t(x) = t(l) Phase delay = j(x) = j(l)

in ( l )
E% out ( l )
E%

grating grating
f f
f f
f f
Fourier transform plane

H ( l ) = t(l ) exp[ij (l )]
We can control both the amplitude and phase of the pulse.
The two masks or spatial light modulators together can yield any
desired pulse!
A Shaped Pulse for
Telecommunications

Ones and
zeros
Ultrafast Laser Spectroscopy: Why?
Most events that occur in atoms and molecules occur on fs and ps time
scales. The length scales are very small, so very little time is required
for the relevant motion.
Fluorescence occurs on a ns time scale, but competing non-radiative
processes only speed things up because relaxation rates add:

1 1 1
= +
ex fl nr

Biologically important processes utilize excitation energy for purposes

other than fluorescence and hence must be very fast.
Collisions in room-temperature liquids occur on a few-fs time scale, so
nearly all processes in liquids are ultrafast.
Semiconductor processes of technological interest are necessarily
ultrafast or we wouldnt be interested.
The simplest ultrafast spectroscopy
method is the excite-probe technique.
This involves exciting the sample with one pulse, probing it with
another a variable delay later, and measuring the change in the
transmitted probe pulse average power vs. delay:

probe pulse
Change in
Probe

energy
pulse

Epr(t)
Sample 0 Delay,
medium
Detector

Variable Eex(t)
delay, Esig(t,)
Excite
pulse

The excite and probe pulses can be different colors.

This technique is also called the pump-probe technique.
Ultrafast Excite-Probe Measurements in DNA
DNA bases undergo photo-oxidative damage, which can yield
mutations. Understanding the photo-physics of these important
molecules may help to understand this process.

Transient absorption at 600 nm of protonated guanosine in acidic

(pH 2) and basic (pH 11) aqueous solution.
Pecourt, et al., Ultrafast Phenomena XII, p.566(2000)
Beyond ultrafast spectroscopy: controlling
chemical reactions with ultrashort pulses
You can excite a chemical bond with the right wavelength, but the
energy redistributes all around the molecule rapidly (IVR).

But exciting with an intense, shaped ultrashort pulse can control the
molecules vibrations and produce the desired products.
Ultrashort in time is also ultrashort in space.
Novel imaging techniques yield ~1-m resolution, emphasizing
edges of objects. They include optical coherence tomography
and multi-photon imaging.

Two-photon fluorescence emission from a focused pulse:

One-photon fluorescence from a

beam entering from the right

Two-photon fluorescence from

an identical beam entering from
the left
SHG and THG Imaging Simultaneously
Images of a Zebrafish larva

20 mm 20 mm

THG (blue) shows edges: the Muscle fibers exhibit strong SHG
larva skin and boundary of (green) due to crystalline nano-
somite and notochord. structure.
Sun and coworkers, Opt. Expr. Nov. 2003
Low-Coherence Reference
Michelson
Interferometry Interferometer
Sample
When the interferometer paths Source
are equal, the intensity fringes
are the strongest. The accuracy Detector
is the coherence time/c.

High-coherence Source Low-coherence Source

l/2
Coherence
Output intensity

Output intensity
Length

Mirror Displacement Mirror Displacement

 OCT Measurements of a Live Tadpole

Dorsal Ventral

Reflectance 1 mm

Boppart, et al., Dev. Biology 177 (1996)