VOLUME 7, NUMBER PHYSICAL REVIEW LETTERS AUGUST 15, 1961

GENERATION OF OPTICAL HARMONICS

P. A. Franken, A. E. Hill, C. %. Peters, and G. Weinreich
The Harrison M. Randall Laboratory of Physics, The University of Michigan, Ann Arbor, Michigan
(Received July 21, 1961)

The development of pulsed ruby optical masers'~' Table I. The square of the total p perpendicular to
has made possible the production of. monochro- the direction of propagation of light through crystal-
matic (6943 A) light beams which, when focussed, line quartz.
exhibit electric fields of the order of 10' volts/cm.
The possibility of exploiting this extraordinary
Direction of incident The square of the total p
intensity for the production of optical harmonics beam perpendicular to direction
from suitable nonlinear materials is most appeal- of propagation
ing. In this Letter we present a brief discussion
of the requisite analysis and a description of ex- —0
p 2+p
2

periments in which we have observed the second 2 4

p g 2+p x ~2y
harmonic (at-3472 A) produced upon projection x
2— 2+1
of an intense beam of 6943A light through crystal- px 2+p ~2(g 2)2
g x
line quartz.
A suitable material for the production of optical
harmonics must have a nonlinear dielectric coef-
ficient and be transparent to both the fundamental (z is the threefold, or optic, axis; x a twofold
optical frequency and the desired overtones. Since axis). If a, light beam traverses quartz in one of
all dielectrics are nonlinear in high enough fields, the three principal directions, Eqs. (2) predict
this suggests the feasibility of utilizing materials the results summarized in Table I. The second-
such as quartz and glass. The dependence of polar- harmonic light should be absent in the first case,
ization of a dielectric upon electric field E may be dependent upon incident polarization in the second
expressed schematically by case, and independent of this polarization in the
third.
I'= yEil+ E +
Y'
— 2+
)i,
~ ~ ~
If an intense beam of monochromatic light is
focussed into a region of volume V, there should
occur an intensity I of second harmonic given
where E„E, ... are of the order of magnitude of
(in Gaussian units) by
atomic electric fields (-10' esu). If E is sinusoi-
dal in time, the presence in Eq. (1) of terms of
quadratic or higher degree will result in P con-
taining harmonics of the fundamental frequency. where ~ is the angular frequency of the second
Direct-current polar izations should accompany harmonic, t." the velocity of light, and v an ef-
the even harmonics. fective "volume of coherence"; that is, the size
Let p be that part of P which is quadratic in E; of a region within the sample in which there is
that is, p is a linear function of the components phase coherence of the p excitation. (This volume
of the symmetric tensor EE. The eighteen coef- may in practice be much smaller than V. ) An
ficients which occur in this function are subject estimate of v is governed by several considera-
to restrictions due to the point symmetry of the tions. For example, it is probably of no greater
medium. These restrictions are, in fact, identi- extent in the propagation direction than - [n,
cal with those governing the piezoelectric coef- x(n, -n, ) ']y„where n, and n, are the indices
ficients. In particular, p necessarily vanishes of refraction for the fundamental and second har-
in a material such as glass which is isotropic or monic frequencies, respectively, and ~, is the
contains a center of inversion. For crystalline wavelength of the second harmonic. The lateral
quartz, however, there are two independent co- extent of this volume is determined in large part
efficients a and P in terms of which by the coherence characteristics of the optical
maser. The situation for a maser of the gas
p X =o(EX2-E ~)+pE E discharge' type is clearly more favorable in
this respect than that for the ruby device. '~ For
P =-PEXE8 -2oE XE
a coherence volume of 10""em, which we think
—0
2
(2) may be realistic in our case, Eq. (1) indicates

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VOLUME 7, NUMBER 4 PHYSICAL RKVIEW LETTERS AUGUST 15, 1961

54 55 38 57 58 39 40 50 55 60 85 70 &5 80
I I II II III IIIIIIIIIIIIIIIIIIIIIIIIIIIIIIIIIIII IIIIIIIIIIIIIIIIIII I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I I II IIIIIIIIIIIII hlII « I I I I I I VI I I II IIIII

FIG. 1. direct reproduction of the first plate in which there was an indication of second harmonic. The
A
wavelength scale is in units of 100 A. The arrow at 3472 A indicates the small but dense image produced by the
second harmonic. The image of the primary beam at 6943 A is very large due to halation.

that second harmonic intensities as high as a us to believe that the order of 10" second har-
fraction of a percent of the fundamental could be monic photons were generated within the quartz
achieved. sample per pulse.
In the experiments we have used a commerci- The production of a second harmonic should
ally available ruby optical maser4 which produces be observable in isotropic materials such as
approximately 3 joules of 6S43A light in a one- glass if a strong bias field were applied to the
millisecond pulse. This light is passed through sample. This bias could be oscillatory, thus
a red filter for the elimination of the xenon flash producing sidebands on the fundamental fre-
background and is then brought to a focus inside quency and the harmonics.
a crystalline quartz sample. The emergent beam We would like to thank the staff of Trion Instru-
is analyzed by a quartz prism spectrometer ments, Inc. , for their valuable and sustained co-
equipped with red insensitive Eastman Type 103 operation in this work.
spectrographic plates. A reproduction of the first
plate in which there was an unambiguous indica-
tion of second harmonic (3472 A) is shown in Fig. *This work was supported in part by the U. S. Atomic
1. This plate was exposed to only one "shot" Energy Commission.
from the optical maser. We believe the following ~T. H. Maiman, Nature 187, 493 (1960).
two facts, among others, rule out the possibility 2R. J. Collins et al. , Phys. Rev. Letters 5, 303
of artifact: (1960) .
(1) The light at 3472 A disappears when the A. Javan, %. R. Bennet, and D. R. Herriott, Phys.
Rev. Letters 6, 106 (1961). Even though the intensity
quartz is removed or is replaced by glass.
of the gas device is very low compared with ruby masers,
(2) The light at 3472 A exhibits the expected the gain in coherence volume and the potential improve-
dependence on polarization and orientation sum- ment of focussing suggest that the gas maser may be
marized in Table I. comparable or even superior as a source for optical
Considerations of the photographic image densi- harmonics.
ty and the efficiency of the optical system lead 4Trion Instruments, Inc. , Model No. TO-3000.

119