IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 46, NO.

6, JUNE 2010

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Two- and Three-Photon Absorption Induced

Emission, Optical Limiting and Stabilization of
CdTe/CdS/ZnS Quantum Tripods System
Guang S. He, Ken-Tye Yong, Jing Zhu, Hai-Yan Qin, and Paras N. Prasad

AbstractTwo- and three-photon absorption and excitation

properties of CdTe/CdS/ZnS quantum tripods in chloroform have
been investigated by using 160-fs laser pulses in the spectral
(11501650) nm. The two- and three-photon excited
range of
up-conversion emission is located around 740-nm position; the
emission intensity follows the square law and cubic law on the
excitation intensity for the former and the latter, respectively.
The nonlinear transmission and output/input characteristics have
been measured at a two-photon absorption wavelength of 1175 nm
and a three-photon absorption wavelength of 1580 nm separately.
Fairly good optical power limiting and stabilization performance
of this material have been achieved.
Index TermsOptical limiting, optical stabilization, nanoparticles, quantum tripods, multi-photon absorption.

I. INTRODUCTION
T IS KNOWN that multi (two, three, or four)-photon absorption (MPA) is one of the best approaches for optical
limiting and stabilization purposes [1], [2]. Optical limiting effect can be used for protecting the human eyes or optical sensors
from laser beam-induced damages; while MPA-based stabilization is highly useful for reducing the temporal and/or spatial
intensity fluctuations of optical signals. So far, most reported
studies for optical limiting and stabilization are based on organic
chromophores, crystals, and polymers, which exhibit large 2PA
cross section values but have a disadvantage in photo-chemical
and photo-physical stability for applications [2]. To date, many
recent efforts have focused on the studies of multi-photon properties of semiconductor nanoparticles, [3][14] as well as on
their applications in frequency upconversion lasing, [15][17]
frequency upconversion imaging, [18][20] and optical power
limiting [21][23]. In comparison with organic multi-photon active materials, inorganic semiconductor nanoparticles may provide the advantages of high photo-chemical and photo-physical
stabilities, and therefore can withstand a higher laser intensity
(and energy) level for power limiting and stabilization applications. In this work, we report the experimental results on the

Manuscript received September 24, 2009; revised December 10, 2009. Current version published March 10, 2010. This work was supported by the Directorate of Chemistry and Life Science of the U.S. Air Force Office of Scientific
Research, Washington DC.
The authors are with the Institute for Lasers, Photonics and Biophotonics,
State University of New York at Buffalo, Buffalo, NY 14260-3000 USA
Color versions of one or more of the figures in this paper are available online
at http://ieeexplore.ieee.org.
Digital Object Identifier 10.1109/JQE.2010.2041325

multi-photon excitation properties of quantum-tripods system

and their application for optical limiting and stabilization.
II. SAMPLES AND EXPERIMENTAL SETUP
The multi-photon active material for this study is
CdTe/CdS/ZnS quantum tripod nanoparticles. CdTe/CdS/ZnS
quantum tripods were prepared by growing a CdS/ZnS graded
shell on a CdTe tripod core [24][27]. Briefly, the reaction
was carried out with CdTe core with tripods corresponding to
0.2 g, using a Cd:Zn:S ratio of 0.2:1:0.4 (1 mmol Cd, 5 mmol
Zn, and 2 mmol S), 10 mL of oleic acid and 5 g of TOPO at
180
C. The quantum tripods were separated from the
surfactant solution by the addition of ethanol and centrifugation. The black precipitate could be readily redispersed in
various organic solvents (hexane, toluene, and chloroform).
The transmission electron microscopy (TEM) image of the
CdTe/CdS/ZnS quantum tripods deposited from organic media
is presented on the top right of Fig. 1(a). The average length
and width of each arm are estimated to be 20 nm and 4 nm,
respectively. The angle between two arms is approximately
120 . Previous studies have shown that the formation of
multi-arms nanocrystals can be achieved using phosphonic
acids that strongly coordinate with Cd atoms, thereby slowing
the nanocrystals growth and resulting in preferential growth in
the c axis direction of the wurtzite crystal structure [28][30].
In this study, similar approach was used to fabricate the
tripod-shape nanocrystals.
The linear absorbance spectra of 1-mm path-length pure solvent (CHCl ) and two CdTe tripods/CHCl samples with different concentration values are shown in Fig. 1(a). The linear
transmission spectra of 1-cm long pure solvent and a tripod
mg/mL concentration are dissolution sample of
played in Fig. 1(b). From these two figures one can see that
there is a strong UV absorption band that is decaying toward
the longer wavelength side, but its absorption tail covers the
whole visible spectral range. For light wavelengths longer than
800 nm and even with a high-concentration sample of tripods in
CHCl , there is no linear absorption at all except several narrow
IR absorption bands that belong to the solvent itself. Therefore,
one may expect that the effective two-photon absorption (2PA)
can take place by using excitation wavelengths in the range of
(8501400) nm, and three-photon absorption (3PA) will occur
in the excitation range of (14501680) nm, respectively.
In our multi-photon excitation experiment, the intense coherent excitation source was an optical parametric generator
(OPG), pumped by 775-nm and 160-fs laser pulses from a

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spectral measurement was reduced to 1 mg/mL. Fig. 2(b)

shows the curves of relative emission intensity dependence on
the excitation pulse energy, measured at 1250-nm and 1630-nm,
respectively. In a double-logarithm scale, the measured data are
well fitted by a straight line with the slope of 2 for the former
and another straight line with the slope of 3 for the latter,
confirming the 2PA and 3PA features at these two excitation
wavelengths. Based on the results shown in Fig. 2(a), one can
conclude that the emission spectral profiles for one-, two- and
three-photon excitation are basically the same with the emission
-nm position and bandwidth of
peak located around
45 nm. On the other hand, it is known that the selection rules
and transition pathways are generally different for the cases
of one-, two-, and three-photon excitation processes. Similar
to what observed in organic multi-photon active chromophore
systems, the results shown in Fig. 2(a) reveal that after one-,
two- or three-photon excitation, the emitting centers of the
tripod particles finally relax to the same energy level(s), and
then emit the same spectra.
IV. 2PA-BASED OPTICAL LIMITING AND STABILIZATION

Fig. 1. (a) Linear absorbance spectra for a 1-mm path-length pure solvent
(CHCl ) sample and two CdTe tripods/CHCl solution samples with different
concentration values. (b) Linear transmission spectra of a 1-cm pure solvent
sample and a 1-cm tripods solution sample of d concentration. The inset in
(a) is the TEM image of the tripods.

Ti-sapphire oscillator/amplifier system (CPA-2010 from ClarkMXR, Inc.) operating at a repetition rate of 1 kHz. The output
wavelength from this OPG could be tuned over the spectral
range from 1100 nm to 1900 nm. The output beam was linearly
polarized with an 3-mm beam size and 0.5-mrad divergent
angle.
III. MULTI-PHOTON INDUCED EMISSION
The CdTe/CdS/ZnS tripods/CHCl solution sample emits
photoluminescence upon exciting the nanoparticles with one-,
two-, and three-photon absorption at suitable wavelengths. As
an example, Fig. 2(a) shows the emission spectra excited by
laser pulses at three different wavelengths, i.e., 625 nm (for
1PA), 1250 nm (for 2PA), and 1630 nm (for 3PA), respectively.
These spectra were recorded by using a grating spectrometer
(EPP 2000 from StellarNet), and the 625-nm excitation beam
was the second-harmonic generation of the 1250-nm pulsed
laser beam. To avoid the reabsorption influence on the emission
spectral profile, the sample concentration for the emission

To quantitatively characterize the multi-photon absorption

properties of our samples and demonstrate their optical power
limiting performance, we have specifically chosen 1175-nm
and 1580-nm wavelengths for the 2PA- and 3PA-induced
nonlinear transmissivity measurements. At these two wavelengths, the linear transmissivity is higher than 90% for the
1-cm path-length samples with two chosen concentration levels
mg/mL and
mg/mL). In both cases, the
-cm
input excitation pulsed laser beam was focused by an
lens into the center of a 1-cm thick sample solution cuvette.
The input and output pulse energy values were measured by
a large-area energy-meter. To avoid thermal lensing influence
on the measurement, the input laser beam was first passed
through a beam chopper with an opening ratio of 1
and a
rotating speed of 75 rounds per second. After passing through
this chopper, the pulse number per second was reduced from
1000 to 150, while the energy or peak power of each individual
pulse remained unchanged.
Fig. 3(a) shows the measured nonlinear transmission versus
the input 1175-nm laser pulse energy for the 1-cm path-length
samples with two different concentration values. According to
the basic 2PA theory, the nonlinear transmission of a one-photon
transparent but two-photon absorbing medium excited by a focused laser beam with a hat-top pulse shape can be expressed as
follows [1]:
(1)
where
is the peak intensity of the input laser beam inside
the medium, is the thickness of the sample, and is the 2PA
coefficient of the medium. In Fig. 3(a) the two groups of experimental data can be well fitted by two theoretical curves given
by (1) with two values, i.e.,
cm/GW for sample
cm/GW for sample of
.
of concentration and
These results are reasonable as the 2PA coefficient is proportional to the concentration of the nonlinearly absorbing nanoparticles. Furthermore, Fig. 3(b) shows the measured data of output

HE et al.: OPTICAL LIMITING AND STABILIZATION OF CdTe/CdS/ZnS QUANTUM TRIPODS SYSTEM

Fig. 2. (a) Normalized emission spectra excited by one-photon absorption at

625 nm, two-photon absorption at 1250 nm, and three-photon absorption at
1630 nm; (b) Measured relative emission intensity versus input pulse energy of
the 1250-nm beam and the 1630-nm beam, showing the quadratic dependence
and cubic dependence respectively.

pulse energy versus the input pulse energy, the theoretical fitting curves with the corresponding values are given by the
following equation:
(2)
where
and
are the input and output pulse energy, respectively. From Fig. 3(a), one can readily find that the nonlinear transmissivity for the high concentration sample is reduced from 1 to 0.2 when the input pulse energy is increased
from 0.1 J to 12 J. This is a typical and efficient power
limiting effect. Also from Fig. 3(b), we can observe that at high
input levels (612 J), a relatively large input pulse energy (intensity) fluctuation will only lead to a much smaller output fluctuation; this is the so-called optical stabilization effect based on
2PA mechanism. Each experimental point shown in Fig. 3 is a
result of average over 100 pulses, the measurement errors are
caused by the input pulse energy fluctuations.

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Fig. 3. (a) Measured nonlinear transmission of two solution samples versus

the input energy or peak intensity of 1175-nm laser pulses. (b) Measured output
pulse energy versus input energy of the same laser beam. The solid- and dashedline are the best fitting curves given by 2PA theory.

Here, for our CdTe/CdS/ZnS quantum tripod sample of

mg/mL concentration, the measured 2PA coefcm/GW. Our previous results obtained
ficient is
under basically the same experimental conditions showed
that for CdSe quantum dots of 4-nm size and 70 mg/mL
cm/GW
concentration in hexane, the measured
(at 775-nm wavelength) [13]. For CdTe quantum dots of
7 nm size and 8 mg/mL concentration in chloroform, the
cm/GW (at 1300-nm wavelength) [23].
measured
Moreover, AF350 dye is among the best two-photon active organic chromophores, at the concentration level of 20 mg/mL in
cm/GW
tetrahydrofuran (THF), its 2PA coefficient is
(at 800 nm) [31].
To further demonstrate the application of this nonlinear
effect, we measured the normalized peak power fluctuation
of the input 1175-nm pulses at an average energy level of
10 J, and the fluctuation of the output pulses after passing
mg/mL concentration.
through the 1-cm sample of
These results are obtained by using a large-area (4 4 mm )
photodetector (SET110 from Thor-Labs) in conjunction with a

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IEEE JOURNAL OF QUANTUM ELECTRONICS, VOL. 46, NO. 6, JUNE 2010

Fig. 4. Displays of the input pulses fluctuation (a) and the output pulses
fluctuation (b) recorded by a high-speed oscilloscope. The input wavelength is
1175 nm, pulse energy 10 J, and the 1-cm solution sample concentration is
24.6 mg/mL.

500-MHz band-width oscilloscope (Infinum from HP). The experimental results are shown in Fig. 4, indicating that the input
relative fluctuation (standard deviation) is 0.24, whereas the
output fluctuation is reduced to 0.13. This is an experimental
evidence for the improvement of stability of femtosecond laser
pulses, based on a nonlinear absorbing nanoparticles system.
V. 3PA-BASED LIMITING AND STABILIZATION
In a similar way, under the condition of 3PA excitation with
1580-nm laser wavelength, the measured nonlinear transmission and output energy as a function of the input energy are
shown in Fig. 5(a) and (b) individually; the same 1-cm long
samples with two different concentration values were employed
for these measurements. According to the basic 3PA theory, the
nonlinear transmissivity can be written as
(3)
where is the 3PA coefficient of the sample medium. It is found
that the experimental data shown in Fig. 5 cannot be simply
fitted by using (3). However, these data can be well fitted by
the modified 3PA theory by considering 3PA saturation effect
[32], according to which the nonlinear transmission upon 3PA
excitation is expressed as
(4)

Fig. 5. (a) Measured nonlinear transmission of two solution samples versus

the input energy or peak intensity of 1580-nm laser pulses. (b) Measured output
pulse energy versus input energy of the same laser beam. The solid- and dashedline are the best fitting curves given by 3PA theory with considering the saturation effect.

Here
is 3PA saturation intensity parameter that is a
is the unsaturated 3PA coefficient
medium constant, and
. It is noted
when the input intensity is much lower than
that the similar saturation behavior of 3PA in CdSe quantum
dots solution system was also previously reported [13]. In
our present case for CdTe tripods/CHCl solution system,
cm /GW for
the best fitting values are
mg/mL sample,
cm /GW for
sample, and
GW/cm for both samples.
value and
Once again, the linear relationship between the
the concentration value holds. In Fig. 5(b), the fitting curves
,
are obtained by using the same relationship of
is given by (4).
where
Upon comparing Fig. 5 to Fig. 3, we can see that in our 3PA
excitation case, the decrease of nonlinear transmission is getGW/cm ) due to the
ting slower at high input levels (
3PA saturation effect, which is undesirable for optical limiting
and stabilization considerations. In Fig. 6, we present the measured fluctuation of the input 1580-nm pulses for 3PA excitation (a) and the output pulse fluctuation of the same beam after
concentration (b). The
passing through the 1-cm sample of

HE et al.: OPTICAL LIMITING AND STABILIZATION OF CdTe/CdS/ZnS QUANTUM TRIPODS SYSTEM

Fig. 6. Displays of the input pulses fluctuation (a) and the output pulses fluctuation (b) recorded by a high-speed oscilloscope. The input wavelength is 1580
nm, pulse energy 9 J, and the 1-cm solution sample concentration is 12.3
mg/mL.

average input pulse energy was 9 J. In spite of the saturation

effect, we still see certain degree of improvement of the output
stability; the standard deviation for input pulses around their average value is 0.31, whereas that for output pulses is reduced to
0.25.
Efficient carrier multiplication in quantum dots has been reported for many nanoparticles including CdSe, PbS, PbSe, and
PbTe. However, very few studies are available on CdTe systems.
In this process, absorption of a single energetic photon leads to
generation of two or more electron/hole pairs. The interest in
this phenomenon arises from the fundamental importance of understanding the role of quantum confinement from the nanocrystals in comparison to the bulk materials. The current studies
of multi-photon excitation properties of our samples and other
semiconductor nanoparticles systems may be helpful for explore other applications. For example, CdTe tripod nanocrystals
might be a good candidate as efficient carrier multiplication for
solar power applications. We speculate that this material will
allow more complete conversion of photon energy into electric
potential through the generation of multiple electronhole pairs.
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Guang S. He is a Senior Research Scientist with the Photonics Research Laboratory, State University of New York at Buffalo, in 1987 and the Institute
for Lasers, Photonics and Biophotonics since 1999. His major research activities cover the areas of laser physics, nonlinear optics, and multi-photon active
materials. His current research efforts are focused on multi-photon excitation
process and novel nonlinear optical materials and devices. He has published
more than 130 scientific articles and co-authored five monographs including
the book Physics of Nonlinear Optics (World Scientific, 2000).

Ken-Tye Yong received the B.S. and Ph.D. degrees from the State University
of New York at Buffalo in 2001 and 2006, respectively.

Currently, he is a Postdoctoral Research Associate in the Institute of Lasers,

Photonics, and Biophotonics at SUNY Buffalo. His research interest is in the
development of nanomaterials for early cancer detection, diseases diagnosis,
and therapy.

Jing Zhu received the B.S. degree in electronic science and engineering from
Southeast University, China, in 2003, where he is now pursuing the Ph.D. degree
in physical electronics.
Currently, he is a visiting research scholar in the Institute for Lasers, Photonics and Biophotonics, State University of New York at Buffalo.

Hai-Yan Qin received the B.S. degree in information engineering from Zhejiang University, Hangzhou, China, in 2005. She is now a joint Ph.D. student
in optical communication technology at Zhejiang University, China, and in
biotechnology at the Royal Institute of Technology, Sweden.
She was a visiting research scholar in the Institute for Lasers, Photonics and
Biophotonics, State University of New York at Buffalo.

Paras N. Prasad is Executive Director of the Institute for Lasers, Photonics and
Biophotonics and a Distinguished Professor of chemistry, physics, medicine and
electrical engineering at the State University of New York at Buffalo. He also
holds the Samuel P. Capen Chair. He has published more than 500 scientific
papers and co-edited 5 books. He co-authored a monograph, Introduction to
Nonlinear Optical Effects in Molecules and Polymers (Wiley) and authored two
recent monographs, Introduction to Biophotonics (Wiley) and Nanophotonics
(Wiley).
Dr. Prasad is a Fellow of the American Physical Society and a Fellow of the
Optical Society of America. He is also a recipient of the prestigious Sloan and
Guggenheim fellowships.