Nonlinear optics produces a

broadband supercontinuum of
light. Self-phase modulation
of light passing through a
highly nonlinear optical fiber
spreads the input light across
the whole visible spectrum.

Courtesy of the University of Bath

34 | OPN Optics & Photonics News www.osa-opn.org

1047-6938/10/11/0034/7-$15.00 OSA
How the Laser Launched
Nonlinear Optics
Jeff Hecht

If the laser was a solution, nonlinear optics was one of the problems it
was seeking. Intense pulses of coherent, monochromatic light were just
what was needed to produce nonlinear effects. Once physicists got their
first lasers, nonlinear optics blossomed in a golden age of discovery.

N onlinear optics was discovered long before the laser, but lasers made the field bloom. The short,
bright, coherent pulses from the ruby laser concentrated light in just the way needed to produce
previously unobservable nonlinear effects. Peter Franken launched a burst of research activity
with his landmark 1961 experiment in which he fired pulses from a rented ruby laser into a quartz crystal at
the University of Michigan.
A spectrograph displayed a large, bright spot at rubys 694-nm fundamental line. In addition, a photo
of the output revealed a faint spot at 347 nm, the ultraviolet second harmonic. In fact, it was so dim that
the lithographer preparing the picture for Physical Review Letters thought it was a flaw and removed it. Yet
it was enough to show that nonlinear effects, already known at radio and microwave wavelengths, could
occur at much higher optical wavelengths.
Other groups soon turned ruby lasers on other materials, sometimes finding nonlinear effects they
hadnt expected, other times verifying theoretical predictions. It was a wonderful example of how physicists
playing with a new toy could expand the frontier of knowledge.

Roots of nonlinear optics

Classical optics respond linearly to light. However, as far back as the 19th century, physicists saw signs
of nonlinear effects as well. In 1875, Scottish physicist John Kerr found that an electric field can polarize
optically isotropic materials, but this quadratic electro-optic effect is too slow to be nonlinear at optical
frequencies. The linear electro-optic effect, described in 1895 by Friedrich Pockels, is much faster, allowing
the electric field of light waves to modulate the refractive index of suitable materials at their own frequency.
That led Nicolaas Bloembergen to call it a true precursor of nonlinear optics.
Russians Sergey Vavilov and Vadim L. Levishin observed the first purely optical nonlinear effect in 1926
when they focused microsecond pulses from a condensed spark to power densities on the order of kilowatts
per square centimeter. Illuminating uranium-doped glass decreased its absorption by 1.5 percent, a change

November 2010 | 35
 Peter Franken
received OSAs
R.W. Wood
prize in 1979
for his work
they attributed to saturation by the intense that led to the that was the first to manufacture ruby lasers.
light. Vavilov, who became a leading development He rented one, and got his Michigan col-
Soviet-era physicist, introduced the term of nonlinear league Wilbur Peters to set up a spectrograph
nonlinear optics in 1944. optics. and camera to measure emitted light. He
By that time, others had also recognized was set to fire the laser at a fused quartz
purely optical nonlinearities. In 1941, Amer- target, which he had picked because it was
ican chemist Gilbert N. Lewis discovered transparent at both the 694-nm fundamental
intense light fluorescence from fluorescein harmonic and the 347-nm second harmonic.
dye in borate glass. Brian OBrien of the Then Weinreich told him they couldnt use
University of Rochesters Institute of Optics OSA Historical Archives
an isotropic material like fused quartz, and
put saturation effects to practical use during instead needed crystalline quartz, which lacks
World War II in the Icaroscope, which he Peter Franken a center of inversion.
devised to counter the Japanese Air Force The experiments were demandingand
practice of attacking with the sun behind launched a burst of not only because they had to haul 50-L dewars
them. The instrument focused the area near research activity with of liquid nitrogen to the fourth floor lab to
the sun onto a phosphor, which the user cool the laser while the elevator was being
viewed instead of looking at the sky. Direct his landmark 1961 repaired. The harmonic conversion efficiency
sunlight saturated the phosphor, but adja-
cent areas remained unsaturated, revealing
experiment in which was extremely low, and alignment require-
ments were demanding, so it took them a long
incoming Japanese bombers. he fired pulses from time to get usable results. Their laser fired
By the postwar years, nonlinear effects three-joule, one-millisecond pulses, containing
at radio and microwave frequencies were a rented ruby laser about 1019 photons, but focusing them into the
well-known thanks to the development of into a quartz crystal crystalline quartz generated at best only about
communications and radar systems. Yet 1011 second-harmonic photons.
scaling to optical wavelengths was far from at the University Nonetheless, their photographic plate
straightforward because light-matter inter- of Michigan. clearly showed the small second harmonic
actions differ strongly between radio and spot. They submitted their paper in mid-July,
optical frequencies. Moreover, the coherent a little over four months after the meeting,
radiation available from radio oscillators was not readily avail- and it appeared in the August 15, 1961, Physical Review Letters.
able at optical frequencies until Theodore Maiman demon- Looking back, it seems an obvious test, but back then it
strated the laser in 1960. Nonetheless, the idea of nonlinearity was revolutionary. At that time, we were all thinking photons,
was lurking in the background as the laser emerged. and you cant change the frequency of a photon, said Fran-
ken. That was what was so revolutionary about the thought
Second-harmonic generation that you could have optical harmonics. Working with Willis
Lamb at Oxford University in 1959 had taught him that clas-
Lasers were hot by early 1961, so the Optical Society of Ameri- sical electromagnetic wave theory applied to optical photons,
ca scheduled laser sessions for its spring meeting in Pittsburgh, so he had realized that nonlinearities might generate optical
held in early March. A packed house listened to a series of laser harmonics. Some visitors to his lab had scoffed at his plans for
talks, but Frankens mind began wandering when they droned second-harmonic generationuntil they worked.
on endlessly about applications in communications and eye The faint second-harmonic spot that never made it into
surgery. Seeking something really unusual, he calculated the print launched modern nonlinear optics in both the United
intensity of a five-kilowatt laser pulse focused onto a 10-m States and Russia. (This article focuses mainly on U.S. work;
spot. His answer was megawatts per square centimeter, with the parallel work in Russia was also impressive and deserves an
electric fields of 100,000 volts per centimeter. article of its own.)
That was just three or four orders of magnitude below the
electric field within an atom, enough to strongly affect or ion-
ize atoms. I realized then that you could do something with Phase matching brightens harmonic generation
it, Franken recalled in a 1985 interview. Further calculations Joe Giordmaine recalls being really struck by Frankens
indicated that the fields should be strong enough to produce results, published just two months after he joined Bell Labs.
detectable amounts of the second harmonic. Excited, he left Don Nelson and Bob Collins had helped him get a ruby laser
the meeting and hurried back to Michigan, where he began up and running, and Giordmaine had begun exploring the
planning an experiment with solid-state physicist Gabriel effects of its very high intensity pulses on materials. So he was
(Gaby) Weinreich. well-prepared to take his own shot at harmonic generation.
Franken was in the right place to find a laser; he was con- Bell had a large stock of crystals left over from World War
sulting for Trion Instruments, a small Ann Arbor company II research on piezoelectric materials. He began testing them,

36 | OPN Optics & Photonics News www.osa-opn.org

and within a few weeks he had not only replicated second-
harmonic generation, but he had produced higher harmonic
power than he had expected from Frankens results. He identi-
fied potassium dihydrogen phosphate (KDP) as a particularly
good nonlinear material, and when he tested crystals cut at
various angles and measured emission in various directions, he
discovered something unexpected. Second-harmonic genera-
tion was not just in the direction of the ruby laser, but also in
an unexpected ring, centered in a different direction. In fact,
second-harmonic generation at certain angles was many times
higher than at others.
He puzzled over that awhile, and eventually realized the
emission peaks came from phase matching of the fundamental
and second-harmonic beams. The crystals were birefringent,
and the second harmonic was polarized orthogonally to the
fundamental. The output was highest when the input beam
was aligned at the angle at which the refractive index was iden-
tical for the fundamental and the second harmonic. That is,
the birefringence of the crystal compensated for the chromatic
dispersion between the fundamental and harmonic.
Phase matching boosted output power a thousand-fold, but
it requires certain crystals. Quartz couldnt be phase-matched,
but birefringent crystals such as KDP could be. Bob Terhune
at the Ford Motor Co. Research Laboratory discovered phase
matching at the same time, and he and Giordmaine both pub-
lished papers in the January 1, 1962, issue of Physical Review
Letters. The phase-matching concept has proved crucial in
optical harmonic generation, but interestingly it has no exact
counterpart in radio engineering.
Nonlinear theory
Frankens paper also stimulated Nicolaas Bloembergen at
Harvard to tackle the theory of nonlinear optics. Bloembergen
had done major work on nuclear magnetic resonance, and he
developed the three-level solid-state maser. When he heard of
Maimans laser, he put two people in his group to work build-
ing different versions of the ruby laser. When he saw a preprint
of Frankens paper, he gathered John Armstrong, Peter Pershan
and Jacques Ducuing to work on nonlinear optics.
Armstrong and Ducuing began experiments, and all four
worked on theory. At the time, Armstrong recalls, physicists
Phase matching in
nonlinear optics.
Courtesy of AT&T Archives and History Center
Nicolaas Bloembergen (left) and
graduate student Pierre Lallemand in
the nonlinear optics lab at Harvard.
Harvard University, courtesy AIP Emilio Segre Visual Archives
in the United States received little or no training in nonlinear
equations, so when Bloembergen wrote down the differential
equations that govern harmonic generation, it was not immedi-
ately obvious what the solution would be.
Nico was the intellectual spark-plug behind the collabora-
tion, Armstrong says. He had a sabbatical in the fall semes-
ter, but he stayed at Harvard. He spent an hour or two each
morning in his office with the group, going through what they
had been working on. Early on, they generalized the prob-
lem beyond harmonic generation to four-wave interactions,
described by a set of seriously nonlinear equations. The group
spent several intense and exciting months, from July to early
1962, dividing elements of the problem among themselves and
working closely with Bloembergen.
The results was a 22-pp. detailed analysis of light interac-
tions in nonlinear dielectrics, drafted in February or March,
submitted in April, and published in Physical Review in
September. It was by no means the last word, but it was a
very complete first word, says Armstrong, whose name was
first in alphabetical order. The mathematics made the paper a
formidable one, but its codification of nonlinear interactions
including harmonic generation and parametric conversion had
a huge impact on the young field.
Stimulated Raman scattering
As Bloembergens group put the final touches on their theo-
retical analysis, experiments with high-power, single-pulse
Q-switched ruby lasers at Hughes Aircrafts Aerospace group
revealed an unexpected nonlinear anomaly.
The Q-switch, invented by Robert Hellwarth of Hughes
Research Labs, produced giant pulses much shorter in
duration and higher in power than previously available. In
early 1962, Eric Woodbury and Won Ng began measuring
November 2010 | 37
laser power with and without a Kerr-cell new wave of excitement. Soon afterwards
1 cm
Q-switch filled with nitrobenzene. Out- Robert Terhune at the Ford Motor Co.
put power was as expected without the Research Laboratory and Boris Stoicheff at
Q-switch, but, with the Q-switch, it seemed the National Research Council of Canada
to be several hundred megawatts, far more pumped Raman-active liquids and produced
than expected. They initially suspected the intense cones of anti-Stokes emission on lines
anomaly came from optical saturation shorter than the laser wavelength.
of the neutral-density filters they used to
avoid overloading their detector. Stimulated Brillouin scattering
They suspected detector problems when and self-focusing
a second experiment also seemed to show
unexpectedly high power in Q-switched Charles Townes bought one of the first
pulses. The lightbulb finally went on Trion ruby lasers when he arrived at MIT
when the researchers added narrow-pass in 1961. The school had hired him as pro-
filters centered on the 694.3-nm ruby vosta largely administrative jobafter
line, and they reduced power to the he had spent two years as vice president and
expected level. Measurements showed research director of the Institute for Defense
Firing a Q-switched ruby pulse Analyses. But Townes set aside some time
their so-called neutral-density filters through an f/20 lens produced
only weakly attenuated the near-infrared, to lead a small research group and teach
a long, thin damage zone that
suggesting that unexpected near-infrared revealed self-trapping. graduate students.
light had muddled their earlier results. Courtesy of Michael Hercher
Analyzing Stoicheffs anti-Stokes data,
Further measurements showed most of Townes realized that when laser light
the extra light was near 750 nm and was The fact that the stimulated Raman scattering, it was gener-
produced only when laser power exceeded ating coherent molecular oscillations that
a threshold reached by Q-switching but
damaged zone was produced the anti-Stokes emission. If lasers
not by normal pulses. A monochroma- smaller than the focal could excite molecular vibrations, Townes
tor identified three near-infrared lines, wondered if they could also stimulate Bril-
the strongest at 766 nm, a weaker line at spotand that it did louin scattering. In just two weeks, graduate
851.5 nm, and a barely detectable line at not increase as the student Ray Chiao, Townes and Stoicheff
demonstrated Brillouin scattering in a solid.
961 nm. The increments appeared roughly
equal in frequency units. At this point, beam passed through Soon another student, Elsa Garmire, dem-
we were convinced that a new form of
laser action had definitely been observed,
the glassled Townes onstrated Brillouin scattering in a liquid.
We also saw other strange phenomena,
and submitted a note to this effect, wrote to suggest that optical such as backward stimulated Brillouin
Woodbury. But they had yet to identify scattering which went into the laser, was
the process. nonlinearities were amplified, and came back out, recalls
Hellwarth and Gisela Eckhardt of offsetting beam Garmire. It would take many years to
Hughes Research Labs suggested the infra- work out all the details. In 1972, Boris Y.
red lines came from stimulated Raman diffraction to cause Zeldovichthe son of noted Soviet nuclear
scattering by the nitrobenzene in the
Q-switch. When Fred McClung replaced
self-trapping. physicist Yakov B. Zeldovichwould show
that stimulated Brillouin scattering could
the nitrobenzene Kerr cell with a Pockels produce phase conjugation.
cell, the infrared lines vanished; however, they reappeared Townes suggested another research direction after seeing
when he put a nitrobenzene cell into the laser cavity. Shining traces made when Michael Hercher of the University of Roch-
long ruby pulses onto a nitrobenzene cell outside the laser cav- ester focused Q-switched ruby laser pulses of a few megawatts
ity produced the same three infrared lines, but they were wider into glass. The traces were filaments of optical damage only
than when pumped by a Q-switched laser, as expected if only a few wavelengths wide that started near the focal point and
Q-switching reached the threshold for stimulated Raman scat- extended up to several centimeters beyond it. The damage was
tering. Hellwarth later developed a full theoretical explanation. surprising, says Robert Boyd of Rochester, because a simple
The accidental discovery of stimulated Raman scattering estimate of the intensity of the incident laser light suggests that
and its identification was another landmark in nonlinear optics. no damage should occur.
Light waves interacted nonlinearly not just with each other, but The fact that the damaged zone was smaller than the focal
also with molecular vibrations to stimulate scattering at Stokes- spotand that it did not increase as the beam passed through
shifted wavelengths longer than the laser line. This created a the glassled Townes to suggest that optical nonlinearities

38 | OPN Optics & Photonics News www.osa-opn.org

were offsetting beam diffraction to cause self-trapping that
concentrated power in the damaged zone. In October 1964,
Chiao, Garmire and Townes described how the intense beam
aligned molecules to create a waveguide within the glass. The
change in refractive index overcame diffraction, trapping the
beam in high-intensity filamentswhich damaged the glass.
Their equations describe what we now call spatial solitons.
Paul Kelley of the MIT Lincoln Laboratory, who was work-
ing with them, wondered how the beam had collapsed. He
used numerical models to develop a theory of self-focusing,
which showed the effect of beam power, scale lengths for
self-focusing, and where the beam collapsed. He worked out
important details, including the scale length for self-focusing,
how it depended on beam power, and where the beam col-
lapsed, in a paper published in December 1965.
Unknown to Kelley or other U.S. researchers, Vladimir
Talanov was working on the same idea in the closed Soviet city of
Gorky. Townes discovered this when he mentioned Kelleys work
to Nikolai Basov and Alexander Prokhorov on a visit to Moscow.
The two Russians invited Talanov to talk to Townes, then had
to get Talanov out of trouble because his research was classified.
Talanov would become an important figure in nonlinear optics.
Soviet research and optical parametric oscillators
By this point, Russia had developed its own vigorous program
in nonlinear optics. Two key figures were Rem V. Khokhlov
and Sergey A. Akhmanov, who founded Russias first non-
linear optics laboratory at Moscow State University in 1962.
That spring, they developed the theory for building an optical
parametric oscillator.
Parametric oscillation was well known at radio frequencies.
However, extending it to optics was an important step because
Courtesy of Moscow State University
Caricature of the two leading figures in Russian nonlinear optics,
Rem Khokhlov (left) and Sergei Akhmanov, celebrating the Lenin Prize
they shared in 1970 for their pioneering work in nonlinear optics.
David Kleinman (left) and Joe
Giordmaine displaying a nonlinear
KDP crystal at Bell Labs.
Courtesy of AT&T Archives and History Center
it could generate tunable output from fixed-wavelength lasers.
Khokhlov and Akhmanov wrote Problems in Nonlinear Optics,
the first book on the topic, published in Russian in 1964 and
in English in 1972. The first edition of Bloembergens Nonlin-
ear Optics appeared in 1965.
The Moscow lab soon developed efficient ways of generat-
ing second, third, fourth and fifth harmonics. A long series of
experiments with Alexander Kovrigin also led to the demon-
stration of an optical parametric oscillator in the spring of
1965, at nearly the same time Giordmaine and crystal expert
Robert Miller demonstrated one at Bell Labs. Both pumped
with the second harmonic of neodymium lasers, with the
Moscow lab using KTP and Bell using lithium niobate as the
nonlinear crystals.
The experiments were not easy. The Russians spent nearly
three years translating their theory into a demonstration.
Giordmaine recalled that his parametric oscillator didnt
produce a pulse every time it was pumped, and its conversion
efficiency was only about 5 percent. However, he could tune
it across 70 nm, an impressive advance in 1965, when tunable
dye lasers had yet to be developed.
A golden age
Ron Shen of the University of California at Berkeley, who
worked with Bloembergen at Harvard, recalls the early years as
a golden age, the beginning of a new field, with a lot of new
effects to be explored. In the late 1960s, researchers explored
the new nonlinear frontier with Q-switched nanosecond ruby
pulses delivering megawatts. Exploration continued in the 1970s
with higher powers and repetition rates from neodymium lasers.
Modelocking generated shorter pulses and higher peak intensi-
ties. And researchers built on the foundation of the early years.
November 2010 | 39

Jim Stone compares the
spectra of supercontinuums
produced when identical
lasers pump two different
nonlinear fibers.
Courtesy of the University of Bath
The concept of self-focusing led to the idea of self-phase-
modulation. Kelley and MIT student Ken Gustafson studied
the generation of shock waves in nonlinear materials. They
found a phase shift that depended on the square of the field
intensity, but, as Kelley recalls, we didnt make a great deal
about it. However, in 1967, Fujio Shimizu at the University
of Toronto demonstrated that in liquids self-phase modula-
tion could spread the spectrum. Once we got started down
this path, we could work out in great detail what people could
observe [from self-phase modulation] and that turned out to be
what they saw, Kelley recalls.
In a 1970 issue of Physics Review Letters, Bob Alfano and
Stan Shapiro at GTE Laboratories in Bayside, N.Y., demon-
strated more frequency spreading in glass and crystals. The
higher the power, the broader the bandwidth, and over the
years the effect spread out the spectrum enough to make
white-light supercontinuums.
In 1973, Akira Hasegawa and F. Tappert took another
important step, extending the concept of self-trapping to
describe optical temporal solitons in optical fibers. Nonlinear
phase modulation and dispersion interact so pulse duration
and frequency chirp increase and decrease periodically along
the length of the fiber, periodically reconstructing the original
pulse. Hasegawa, Linn Mollenauer, and others later showed
solitons could transmit signals through fiber-optic cables.
Modern nonlinear optics
Modern nonlinear optics has come a long way from its roots,
yet the fundamental groundwork remains solid. To this
day, every time I make a discovery in nonlinear optics, I look
at [Bloembergens] paper and hes done it, says Boyd. He
put the whole field together in 18 months. That feat earned
Bloembergen the 1981 Nobel Prize in Physics.
40 | OPN Optics & Photonics News
Nonlinear optics has come so far that its quietly embed-
ded in consumer products. Second-harmonic generation is
at the heart of green laser pointers, which are diode-pumped
neodymium laser frequency doubled to 532 nm. Its hard to
believe you can buy these things, says Garmire. If you think
of whats inside, its just amazing. Corning has developed a
more compact version for use in microprojectors to be built
into smart phones. Yet harmonic generation also finds cutting-
edge laboratory applications, generating pulses of attosecond
duration or with wavelengths in the extreme ultraviolet or
X-ray bands.
Self-phase modulation can spread light across the spectrum.
Its inherently chirped, so pulses can be sent through a medium,
then collapsed to make femtosecond pulses. Add an amplifica-
tion stage where the pulse is dispersed in time, and the resulting
ultrashort pulse can have extremely high peak power. Femtosec-
ond frequency combs are another extension of the concept.
Long transmission distances make nonlinearities inevitable
in fiber-optic communications systems. Stimulated Raman
scattering can be put to good use in amplifying signals or
shifting their wavelengths, but other nonlinearities such as
four-wave mixing challenge system designers trying to control
noise. The more we try to do with optics, the more we have
to think about nonlinearities. Like the laser, nonlinear optics
seem to be everywhere. t
Jeff Hecht (jeff@jeffhecht.com) is a science and technology writer
Member based in Auburndale, Mass., U.S.A.
[ References and Resources ]
>> Nicolaas Bloembergen, oral history interview: www.aip.org/history/
ohilist/4511.html
>> Peter Franken, oral history interview: www.aip.org/history/
ohilist/4612.html
>> Elsa Garmire, oral history interview: www.aip.org/history/
ohilist/4621.html
>> Joe Giordmaine, oral history interview: www.ieeeghn.org/wiki/
index.php/Oral-History:Joseph_Giordmaine
>> Charles Townes, oral history interview (session 1): www.aip.org/
history/ohilist/4917_1.html
>> R.W. Boyd. The Impact of Charles H. Townes on Nonlinear Optics,
IEEE J. Sel. Top. Quantum Electron. 6, 881-4 (Nov/Dec 2000).
>> P.A. Franken et al. Generation of Optical Harmonics, Phys. Rev.
Lett. 7, 118 (1961).
>> J.A. Armstrong et al. Interactions between light waves in a nonlin-
ear dielectric, Phys. Rev. 127(6), 1918-39 (1962).
>> E.J. Woodbury. Raman laser action in organic liquids, 1577-88 in
P. Grivet and N. Bloembergen, Quantum Electronics: Proceedings
of the Third International Congress, Dunot Editeur and Columbia
University Press, 1964.
>> N. Bloembergen. Nonlinear optics: past, present, and future,
IEEE J. Sel. Top. Quantum. Electron. 6, 876-80, Nov/Dec 2000.
>> R.W. Boyd. History of Research in Nonlinear Optics at the Institute
of Optics, Chapter 56 in Carlos R. Stroud ed., The Jewel in the
Crown, Meliora Press, Rochester, 2004, pp. 293-300.
>> R.Y. Chiao et al. Self-focusing of optical beams, in R.W. Boyd
et al., eds, Self-Focusing: Past and Present, Springer, Berlin and
Heidelberg, 2009.
>> E. Garmire. Contributions of Charles Townes research into non-
linear optics, Journal of Laser Applications 21, 208-23 (2009).
www.osa-opn.org