Measuring Ultrashort Laser Pulses

1. Background, Phase Retrieval, and Autocorrelation

2. Frequency-Resolved Optical Gating
3. Interferometric Methods

Rick Trebino
School of Physics
Georgia Institute of Technology
Atlanta, GA 30332 USA

These slides are available at http://public.me.com/ricktrebino.

The vast majority of humankind’s 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.

λ→

Interferometry led to relativity.

And technologies, from medical imaging to

GPS, result from light measurement!
 Most light is broadband, and hence
ultrafast, and also highly complex.
Complex pulse
Ultrafast and complex in time
Intensity

Ultrabroadband supercontinuum

Phase
Arbitrary waveforms

Time

" in time and space

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

We’ll learn much by measuring such light pulses.

Why measure light with ultrafast variations?
To determine the temporal resolution of an experiment using it.

To determine whether a pulse can be

made even shorter. Excitation to excited state
Emission
To better understand the lasers that Excited
emit them and to verify models state
of ultrashort pulse generation.

To better study media: the better Ground state

we know the light in and light
out, the better we know the
medium we study with them.
To use shaped pulses to control
chemical reactions: Coherent control.
Because it’s there.
As a molecule dissociates,
its emission changes color
(i.e., the phase changes),
revealing much about the
molecular dynamics, not avail-
able from the mere spectrum,
or even the intensity vs. time.
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 that’s 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 on9

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

The shortest events ever created are
ultrashort laser pulses.

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

So how do you measure the pulse itself?

You must use the pulse to measure itself.

But that isn’t good enough. It’s only as short as the pulse. It’s not shorter.
 Measuring Ultrashort Laser Pulses I:
Background, Phase Retrieval, and
Autocorrelation
The dilemma
The goal: measuring the intensity and phase vs. time (or frequency)
Why?
The Spectrometer and Michelson Interferometer
1D Phase Retrieval

Intensity Autocorrelation
1D Phase Retrieval
Single-shot autocorrelation
The Autocorrelation and Spectrum
Ambiguities
Third-order Autocorrelation
Interferometric Autocorrelation
 A laser pulse has an intensity and phase
vs. time or frequency.
Its electric field can be written:

{ }

Phase, φ(t)
Intensity, I(t)
E (t ) = Re I (t ) exp [i (ω0t − φ (t ))]
Intensity Phase
Time

Alternatively, in the frequency domain:

Spectrum, S(ω)
E% (ω ) = S (ω ) exp [ −iϕ (ω )]

phase, ϕ(ω)
Spectral
Spectrum Spectral
Phase Frequency

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

phase.
The phase determines the pulse’s
frequency (i.e., color) vs. time.

Example: Linear chirp The instantaneous frequency:

ω (t ) = ω0 − dφ / dt
Phase, φ(t)

time

Light electric field

Frequency, ω(t)

time
time
Time
The spectral phase also yields a pulse’s
color evolution: the group delay vs. ω.
Example: Linear chirp The group delay:

τ g (ω ) = dϕ / dω
phase, ϕ(ω)
Spectral

The group delay vs. frequency is

approximately the inverse of the
frequency instantaneous frequency vs. time.
delay, τg(ω)
Group

We’d like to be able to measure,

not only linearly chirped pulses,
but also pulses with arbitrarily complex
frequency phases and frequencies vs. time.
time
Pulse Measurement in the Frequency Domain:
The Spectrometer
The spectrometer measures the spectrum, of course. Wavelength varies
across the camera, and the spectrum can be measured for a single pulse.

Broad-
Entrance
band Slit Collimating
pulse Mirror

“Czerny-Turner”
Grating
arrangement

Focusing
Mirror
Camera or
Linear Detector Array
One-dimensional phase retrieval
It’s more interesting than it appears

Spectrum, S(ω)

phase, ϕ(ω)
to ask what we lack when we know

Spectral
only the pulse spectrum S(ω).

Recall: E% (ω ) = S (ω ) exp [ −iϕ (ω )] Frequency

Obviously, what we lack is the spectral phase ϕ(ω).

time

Retrieving it is called the 1D phase retrieval problem.

Even with extra information,

it’s 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: Detectors
Detectors are devices that emit electrons in response to photons.

Examples: Photo-diodes, Photo-multipliers

Detector
Detector
Another symbol
for a detector:

Detectors have very slow rise and fall times: ~ 1 nanosecond.

As far as we’re concerned, detectors have infinitely slow responses.

They measure the time integral of the pulse intensity from –∞ to +∞:
∞

∫
2
Vdetector ∝ E (t ) dt
−∞

The detector output voltage is proportional to the pulse energy (or fluence).
By themselves, detectors tell us little about a pulse.
Pulse Measurement in the Time Domain:
Varying the pulse delay
Since detectors are essentially infinitely slow, how do we make time-
domain measurements on or using ultrashort laser pulses?

We’ll delay a pulse in time. Input

Mirror pulse E(t)
And how will we do that? Output
By simply moving a mirror! pulse E(t–τ)
Translation stage

Moving a mirror backward by a distance L yields a delay of:

Do not forget the factor of 2!
τ = 2 L /c Light must travel the extra distance
to the mirror—and back!

Since light travels 300 µm per ps, 300 µm of mirror displacement

yields a delay of 2 ps. This is very convenient.
We can also vary the delay using
a mirror pair or corner cube.
Mirror pairs involve two E(t) Input
reflections and displace pulse
Mirrors
the return beam in space: Output
But out-of-plane tilt yields E(t–τ) pulse
a nonparallel return beam.
Translation stage

Corner cubes involve three reflections and also displace the return
beam in space. Even better, they always yield a parallel return beam:

Apollo 11
Hollow corner cubes avoid propagation through glass.
Pulse Measurement in the Time Domain:
The Michelson Interferometer Input
The detected voltage will be: pulse
VMI (τ )
∞ E(t)
VMI (τ ) ∝ ∫
2
E (t ) − E (t − τ ) dt Mirror
−∞
∞ Beam- E(t–τ) Slow
=∫
2 2
E (t ) + E (t − τ ) − 2 Re[ E (t ) E (t − τ )] dt
*
splitter detector
−∞
Delay
∞
∝ Pulse Mirror
VMI (τ ) ∝ 2∫
2
E (t ) dt energy
−∞
∞
− 2 Re ∫ E (t ) E *(t − τ ) dt
“Interfer-
−∞ ogram”

VMI(τ)
Field autocorrelation: Γ(2)(τ). Looks
⇒
interesting, but the Fourier transform of 0 Delay
Γ(2)(τ) is just the spectrum!
Measuring the interferogram is equivalent to measuring the spectrum.
Can we use these methods to measure a pulse?

Result: Using only time-independent, linear components, complete

characterization of a pulse is NOT possible with a slow detector.

Translation: If you don't have a detector or modulator that is fast

compared to the pulse width, you CANNOT measure the pulse
intensity and phase with only linear measurements, such as a
detector, interferometer, or a spectrometer.

V. Wong & I. A. Walmsley, Opt. Lett. 19, 287-289 (1994)

I. A. Walmsley & V. Wong, J. Opt. Soc. Am B, 13, 2453-2463 (1996)

We need a shorter event, and we don’t have one.

But we do have the pulse itself, which is a start.
And we can devise methods for the pulse to gate itself using
optical nonlinearities.
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)(τ).
Pulse to be
measured

The signal field is E(t) E(t-τ).

SHG
Beam So the signal intensity is I(t) I(t-τ)
splitter crystal

E(t–τ) SHG
crystal Detector

Esig(t,τ)
Variable E(t)
delay, τ
∞
The Intensity A(2) (τ ) ≡ ∫ I (t )I ( t −τ ) dt
Autocorrelation:
−∞
Gaussian Pulse and Its Autocorrelation

Pulse Autocorrelation

  2 ln2t  2    2 ln2τ 

2

I (t ) = exp −  FWHM   (2 )
A (τ ) = exp −  FWHM  
  ∆τ p     ∆τ A  

∆τ FW
p
HM

∆τ A
F WH M

t τ

1.41 ∆τ pFWHM = ∆τ AFWHM

Sech2 Pulse and Its Autocorrelation
Pulse Autocorrelation
(2 )
A (τ ) =
1.7627t   2.7196τ
I(t ) = sech  FWHM 
2 3  2.7196τ  
 ∆t p   2.7196τ   ∆τ FWHM coth  ∆τ FWHM  − 1
sinh 2  FWHM   A A 
 ∆τ A 

∆τ FW
p
HM

∆τ A
FW HM

t τ
1.54 ∆τ pFWHM = ∆τ AFWHM

Since theoretical models of ultrafast lasers often predict sech2 pulse

shapes, people usually simply divide the autocorrelation width by 1.54
and call it the pulse width. Even when the autocorrelation is Gaussian9
The Intensity Autocorrelation is always
symmetrical with respect to delay.
This is easy to show:

∫ ∫
A(2) (τ ) = I (t ) I (t − τ ) dt = I (t ′ + τ ) I (t ′) dt ′ = A(2) (−τ )

t′ = t − τ

⇒ A(2) (τ ) = A(2) (−τ )

This means that intensity autocorrelation cannot tell the direction of

time of a pulse. This is, however, a trivial ambiguity—not a big deal.
It’s known, not usually a problem, and easy to remove.
Of course, autocorrelation says nothing about the pulse phase either.
Autocorrelations of more complex intensities
Autocorrelations nearly always have considerably less structure
than the corresponding intensity.

Intensity Autocorrelation
Autocorrelation

Intensity Autocorrelation
Ambiguous Intensity Ambiguous Autocorrelation

-40 -30 -20 -10 0 10 20 30 40 -80 -60 -40 -20 0 20 40 60 80

Time Delay

An autocorrelation typically corresponds to many different intensities.

Thus the autocorrelation does not uniquely determine the intensity.
Even nice autocorrelations have ambiguities.

These complex intensities have nearly Gaussian

autocorrelations.

Intensity Autocorrelation

Autocorrelation
Intensity Ambig Autocor
Ambiguous Intensity Gaussian

-80 -60 -40 -20 0 20 40 60 80 -150 -100 -50 0 50 100 150

Time Delay

Autocorrelation has many nontrivial ambiguities! They’re unknown,

usually a serious problem, and impossible to remove.
Retrieving the intensity from the intensity
autocorrelation is also equivalent to the
1D Phase-Retrieval Problem!
A(2) (τ ) = ∫ I (t ) I (t − τ ) dt
Applying the Autocorrelation Theorem:
2
F { A (τ )} =
(2)
F {I (t)}

Thus, the autocorrelation yields only the magnitude of the Fourier

Transform of the Intensity. It says nothing about its phase!

It’s the 1D Phase-Retrieval Problem again!

We do have additional information: I(t) is always positive.

The positivity constraint removes many nontrivial ambiguities.

But many remain, and no one knows how to find them.

 Autocorrelation of Very Complex Pulses
As the intensity Intensity Autocorrelation
increases in
complexity, its Γ(2)(t)
autocorrelation
approaches a
broad smooth
background and a
coherence spike.

This shows why

retrieving the
intensity from the Ienv(t)
autocorrelation is
fundamentally
impossible!
x intens ities with G aus sian s low ly v arying
2 ∞
A (τ ) = Γ (τ ) + ∫ I (t ) I env (t − τ ) dt
(2) (2)
−∞ env
Geometrical distortions in autocorrelation
When crossing beams at an angle, the delay varies across the beam.

x
Pulse #1 Here, pulse #1 arrives
earlier than pulse #2
Here, pulse #1 and pulse #2
arrive at the same time
Here, pulse #1 arrives
later than pulse #2
Pulse #2
SHG crystal

This effect causes a range of delays to occur at a given time and could
cause geometrical smearing, that is, a broadening of the
autocorrelation in multi-shot measurements.
Single-shot autocorrelation
Crossing beams at an angle also maps delay onto transverse position.

τ ( x) = 2( x / c) sin(θ / 2) ≈ xθ / c

Long pulse Short pulse

x x
SH SH

Use a large beam and a large beam crossing angle to achieve the
desired range of delays. Then image the crystal onto a camera.
So single-shot SHG AC has no geometrical smearing!
Second harmonic generation bandwidth
We need to generate SH for all wavelengths in the pulse.
But the generated SH wavelength depends on angle.
And its angular width varies inversely with the crystal thickness.

Thick crystal creates too narrow a SH

spectrum in a given direction and so
can’t be used for an autocorrelator.

Thick SHG
crystal

Very thin crystal creates a broad SH

spectrum in the forward direction.
Autocorrelators require such very thin
crystals.

Very thin
SHG crystal
 L = 10 µm
The SHG crystal
bandwidth must
exceed that of the
pulse.
L = 100 µm
The SHG bandwidth is usually called
the phase-matching bandwidth.

SHG efficiency vs. wavelength for

the nonlinear-optical crystal, beta-
barium borate (BBO) for different
crystal thicknesses (L): L = 1000 µm

The SHG bandwidth scales as 1/L,

while the efficiency scales as L2.
A nasty trade-off.
Third-order Autocorrelation
Some ambiguity problems in autocorrelation can be overcome by
using a third-order nonlinearity, such as the Optical Kerr effect.

Pulse to be This arrangement is called

measured
Polarization Gating.

Beam Esig(t,τ) = E(t) |E(t-τ)|2

splitter
45° Isig(t,τ) = I(t) I(t-τ)2
E(t-τ) polarization
rotation

Variable E(t) Nonlinear

delay, τ medium (glass) Note the 2

The third-order autocorrelation is not ∞

(τ ) ≡ ∫ I (t ) I ( t −τ )
(3) 2
symmetrical, so it yields slightly more A dt
information, but still not the full pulse. −∞
When a shorter reference pulse is available:
The Intensity Cross-Correlation
If a shorter reference pulse is available (it need not be known), then it
can be used to measure the unknown pulse. In this case, we perform
sum-frequency generation, and measure the energy vs. delay.
SFG
E(t) crystal Slow
Unknown pulse detector
Vdet (τ ) ∝ C (τ )
Reference Eg(t–τ)
gate pulse Lens ESF (t,τ ) ∝ E(t)E g (t − τ )
Delay ⇒ I SF (t ,τ ) ∝ I (t ) I g (t − τ )

The Intensity Cross-correlation: C(τ ) ≡ ∫ −∞

I(t) I g (t − τ ) dt

If the reference pulse is much shorter than the unknown pulse, then the
intensity cross-correlation fully determines the unknown pulse intensity.
Interferometric Autocorrelation
What if we use a collinear beam geometry, and allow the autocorrelator
signal light to interfere with the SHG from each individual beam?

Input
Michelson SHG
pulse Filter Slow
Interferometer Lens crystal
detector
E(t)
Mirror
Beam- E(t–τ) [ E (t ) − E (t − τ )] 2
splitter E (t ) − E (t − τ )
Delay ∞

∫
2 2
Mirror IA (τ ) ≡
(2)
[ E (t ) − E (t − τ )] dt
−∞

New Usual
terms Autocor-
∞

∫
2 relation
IA (τ ) ≡
(2)
E (t ) + E (t − τ ) − 2 E (t ) E (t − τ )
2 2
dt
−∞ term

Also called the Fringe-Resolved Autocorrelation

Interferometric Autocorrelation Math
The measured intensity vs. delay is:
∞

IA(2) (τ ) ≡
∫ −∞
 E 2 (t ) + E 2 (t − τ ) − 2 E (t ) E (t − τ )   E *2 (t ) + E *2 (t − τ ) − 2 E * (t ) E * (t − τ )  dt

Multiplying this out:

∞

IA (τ ) =
(2)
{
∫ E (t −τ ) E (t) + E (t −τ ) − 2E (t −τ )E (t)E (t −τ ) +
−∞ 2
2 2
E (t ) + E (t ) E (t − τ ) − 2 E (t ) E (t ) E (t − τ ) +
*2
2 *2

2 2
2

2
* *

* *

−2 E (t ) E (t − τ ) E *2 (t ) − 2 E (t ) E (t − τ ) E *2 (t − τ ) + 4 E (t )
2
E (t − τ )
2
} dt
∞

=
∫ −∞
{I 2
(t ) + E 2 (t ) E *2 (t − τ ) − 2 I (t ) E (t ) E * (t − τ ) +
E 2 (t − τ ) E *2 (t ) + I 2 (t − τ ) − 2 I (t − τ ) E *(t ) E (t − τ ) +
− 2 I (t ) E (t − τ ) E *(t ) − 2 I (t − τ ) E (t ) E * (t − τ ) + 4 I (t ) I (t − τ )} dt
2
where I(t) ≡ E(t)
 The Interferometric Autocorrelation is the
sum of four different quantities.
∞
=
∫
−∞
I 2 (t ) + I 2 (t − τ ) dt Constant (uninteresting)

∞
+ 4
∫ −∞
I (t ) I (t − τ ) dt Intensity autocorrelation

∞ Sum-of-intensities-weighted ω

∫
− 2 [ I (t ) + I (t − τ ) ] E (t ) E * (t − τ ) dt + c.c “interferogram” of E(t) ω
−∞ (oscillates at ω in delay)
∞ Interferogram of the SH;
+
∫ E (t ) E (t − τ ) dt + c.c.
2 2*
equivalent to the SH spectrum
−∞ (oscillates at 2ω in delay)

The interferometric autocorrelation simply combines several measures

of the pulse into one (admittedly complex) trace. Conveniently, however,
they occur with different oscillation frequencies: 0, ω, and 2ω.
 Interferometric Autocorrelation: Examples

7-fs sech2 800-nm pulse

Pulse with cubic spectral

phase

Double pulse
Interferometric Autocorrelation also has ambiguities.
Pulse #1 Pulse #2
Intensity

Phase

tFWHM = Phase tFWHM=

7.4 fs Intensity 5.3 fs
-40 -20 0 20 40 -40 -20 0 20 40

Interferometric #1 and #2
Chung
Autocorrelations and
for Pulses Weiner,
IEEE
#1 and #2: JSTQE,
2001.

Despite very different pulse lengths, these pulses have nearly identical IAs!
Interferometric Autocorrelation of a
complex pulse
Its Interferometric
Complex pulse Autocorrelation
1 40 8

0.8
6

Intensity (a.u)
Intensity (a.u)

20

Phase (rad)
0.6
4
0
0.4
2
0.2 -20

0 0
-20 -10 0 10 20 -10 0 10
Delay (fs) Delay (fs)

Note that almost all the information in the pulse is missing from its
interferometric autocorrelation. Thus there are also many nontrivial
ambiguities in interferometric autocorrelation, and it is also
fundamentally impossible to retrieve a pulse from its IA.
Quiz: Which is the most difficult?

A. Time travel

B. World peace

C. Human teleportation

D. Retrieving a pulse from its intensity autocorrelation

or interferometric autocorrelation

The correct answer is D. Only it has been proven to be

fundamentally impossible. The others are hard, but,
as far as we know, they may be possible.