1042 IEEE JOURNAL OF SELECTED TOPICS IN QUANTUM ELECTRONICS, VOL. 14, NO.

4, JULY/AUGUST 2008
Interband and Intersubband Optical Properties
of Doped n-Zn
0.46
Cd
0.54
Se/Zn
0.24
Cd
0.25
Mg
0.51
Se
Multiple Quantum Wells for Intersubband
Device Applications
Xuecong Zhou, Sheng-Kun Zhang, Wubao Wang, Robert R. Alfano, Fellow, IEEE, Hong Lu, Maria C. Tamargo,
Aidong Shen, C. Y. Song, and H. C. Liu
AbstractTwo heavily doped n-type Zn
0.46
Cd
0.54
Se/Zn
0.24
Cd
0.25
Mg
0.51
Se multiple quantum well (MQW) structures have
been grown on InP (0 0 1) substrates by molecular beam epitaxy.
Photoluminescence (PL), time-resolved PL, and Fourier transform
infrared (FTIR) spectroscopy were performed to characterize their
interband and intersubband (ISB) properties. These two MQW
samples have similar structures except for different well widths and
a different number of periods. Excitation-intensity-dependent PL
shows no electronic coupling between the multiquantumwells. The
integratedPLintensities andthe PLdecay times of the MQWs were
measured as functions of temperature in the range from 77 to 290
K. Theoretical ttings of temperature dependences of integrated
PL intensities and PL decay times indicate that the nonradiative
recombination processes observed in our samples can be well de-
scribed by hole capture by acceptor-like defect centers through
multiphononemissions. ISBabsorptionspectra of the samples were
measured by FTIR and show peak absorption at wavelengths of
3.99 and 5.35 mfor the MQWs with well widths of 28 and 42

A, re-
spectively. Theoretical calculations based on the envelope function
approximation conrm that these peaks are due to the transitions
from the ground state E
1
to the rst excited state E
2
.
Manuscript received December 1, 2007; revised February 25, 2008. This
work was supported in part by the National Aeronautics and Space Adminis-
tration under Grant NCC-1-03009, in part by the Department of Defense under
Grant W911NF-04-1-0023, and in part by the National Science Foundation
under Grant EEC-0540832 (MIRTHE-ERC).
X. Zhou was with the Department of Physics, Institute for Ultrafast Spec-
troscopy and Lasers, The City College of The City University of New York,
New York, NY 10031 USA. She is now with the HORIBA Jobin Yvon, Inc.,
Edison, NJ 08820 USA (e-mail: cong999@yahoo.com).
S.-K. Zhang is with the Department of Physics, New York City College
of Technology, The City University of New York, Brooklyn, NY 11201 USA
(e-mail: skzhang@citytech.cuny.edu).
W. Wang and R. R. Alfano are with the Department of Physics, Institute
for Ultrafast Spectroscopy and Lasers, The City College of The City Univer-
sity of New York, New York, NY 10031 USA (e-mail: wwang@sci.ccny.cuny.
edu; ralfano@sci.ccny.cuny.edu).
H. Lu was with the Department of Chemistry, The City College of The City
University of New York, New York, NY 10031 USA. She is now with the De-
partment of Materials, University of California at Santa Barbara, Santa Barbara,
CA 93106-5050 USA (e-mail: luhong@engineering.ucsb.edu).
M. C. Tamargo is with the Department of Chemistry, The City College
of The City University of New York, New York, NY 10031 USA (e-mail:
tamar@sci.ccny.cuny.edu).
A. Shen is with the Department of Electrical Engineering, The City Col-
lege of The City University of New York, New York, NY 10031 USA (e-mail:
aidong@sci.ccny.cuny.edu).
C. Y. Song and H. C. Liu are with the Institute for Microstructural Sciences,
National Research Council, Ottawa, ON K1A 0R6, Canada (e-mail: h.c.liu@
nrc-cnrc.gc.ca).
Color versions of one or more of the gures in this paper are available online
at http://ieeexplore.ieee.org.
Digital Object Identier 10.1109/JSTQE.2008.920317
Index TermsIRspectroscopy, optical spectroscopy, photolumi-
nescence (PL), semiconductor epitaxial layers.
I. INTRODUCTION
T
HE advantages of quantum well infrared photodetectors
(QWIPs) over conventional InSb and HgCdTe IRdetectors
include the mature material growth and processing technolo-
gies, which lead to high uniformity, excellent reproducibility,
and thus, large-area, low-cost staring arrays [1], [2]. In addition,
the ability to accurately control the band structure, and hence
spectral response, allows monolithically integrated multispec-
tral IR detectors [3]. The possibility of using multiple quantum
well (MQW) instead of single QW to achieve stronger optical
absorption was rst suggested by Esaki and Sakaki [4], and
the rst experimental measurement of the strong intersubband
(ISB) absorption in a series of MQWs was performed by West
and Eglash [5]. Furthermore, ISB transitions in MQWs have
been receiving considerable attention because of their attractive
optical properties, such as large oscillator strength [5], strong
nonlinearity [6], and fast relaxation processes [7].
Recently, ZnCdSe/ZnCdMgSe MQWs grown lattice-
matched to InP have been recognized as very promising materi-
als to fabricate ISB devices such as mid-IR photodetectors and
quantum cascade lasers (QCLs). These structures have impor-
tant applications in biological and chemical detections. The ISB
transition in these materials covers a wide IR wavelength range
with short wavelength limit less than 2 m. By adjusting the
ux ratios of Zn, Cd, and Mg, Zn
x
Cd
y
Mg
(1xy)
alloys could
be grown lattice-matched to InP substrate by molecular beam
epitaxy (MBE) with bandgap ranging from 2.2 to 3.5 eV [8].
QW structures with large bandgap Zn
x
Cd
y
Mg
(1xy)
Se as the
barrier layer and Zn
x
Cd
(1x)
Se as the well layer have been
grown with emissions ranging from red to blue [8], [9] covering
the whole visible spectra. Based on this materials system, full-
color light emitting diodes [10] and blue-green lasers [11] have
been made. Recently, this system has been reported to have a
very large conduction band offset (CBO), which is found to be
0.59 eV for Zn
0.53
Cd
0.47
Se/Zn
0.29
Cd
0.24
Mg
0.47
Se [12] and
1.12 eV for Zn
0.50
Cd
0.50
Se/Zn
0.13
Mg
0.87
Se [13]. This large
CBO makes the ZnCdSe/ZnCdMgSe system very promising
for optoelectronic device applications based on ISB transitions
such QWIPs and QCL, where large CBO is preferred in order
to obtain the appropriate ISB transitions. For QCL, the strong
1077-260X/$25.00 2008 IEEE
ZHOU et al.: INTERBAND AND INTERSUBBAND OPTICAL PROPERTIES 1043
Fig. 1. Layer structure of the Zn
0. 46
Cd
0. 54
Se/Zn
0. 24
Cd
0. 25
Mg
0. 51
Se
MQW samples.
connement of electrons in QWs provided by the large CBO is
desired for room temperature (RT) operation.
For the optoelectronic device applications, the material prop-
erties especially the optical properties are crucial. In this
paper, interband and ISB optical properties of two n-type
doped Zn
0.46
Cd
0.54
Se/Zn
0.24
Cd
0.25
Mg
0.51
Se MQW struc-
tures grown by MBE on (0 0 1) InP substrates were investi-
gated. Photoluminescence (PL) and time-resolved PL (TRPL)
were used to characterize the interband transition. In addition,
Fourier transform infrared (FTIR) spectroscopy was used to
characterize the ISB transition. Theoretical ttings of the tem-
perature dependences of the integrated PL intensities and PL de-
cay times indicate that the nonradiative recombination processes
observed in our samples can be well described by hole capture
by acceptor-like defect centers through multiphonon emissions
(MPEs). RT FTIR measurements give absorption peaks of 3.99
and 5.35 m for the MQWs with well widths of 28 and 42

A,
respectively. These mid-IR wavelengths are important for the
IR photodetector applications.
II. EXPERIMENTAL METHODS
The two MQW samples were grown by MBE on epi-ready
(0 0 1) InP semiinsulating substrate. The detailed growth
procedure could be found elsewhere [14]. The structure of
the samples is shown in Fig. 1. On top of the InP sub-
strate, an In
0.5
Ga
0.5
As buffer layer (0.15 m), and then,
a Zn
0.46
Cd
0.54
Se layer (0.35 m) was grown, followed by
MQW structures where Zn
0.46
Cd
0.54
Se QWs are sandwiched
between Zn
0.24
Cd
0.25
Mg
0.51
Se barrier layers with thicknesses
of 100 nm. Finally, a thin cap layer of Zn
0.46
Cd
0.54
Se (0.1
m) was grown to protect the Mg from oxidation. The two
samples have similar structures except that the QW width is
42

A for sample A and 28

A for sample B, and the period
number of QWs is 60 for sample A and 80 for sample B. The
Fig. 2. PL spectra at 77 K for sample A (42

A well width, dashed line) and
sample B (28

A well width, solid line).
n-type doping in the QW region was achieved using ZnCl
2
as
dopant and the doping level was measured by Hall effect for
a calibration sample of Cl doped Zn
0.46
Cd
0.54
Se to be about
2 10
18
cm
3
.
Steady-state PL measurements were performed using 325
nm continuous-wave output of a HeCd laser as the excitation
source. TRPL measurements were performed using second har-
monic output (400 nm, 100 fs) of Ti:Sapphire femtosecond laser
as excitation. The emission from the QW samples was selected
by a narrow-band lter and measured using a streak camera
(Hamamatsu Model C5680) at speed 3 with a time resolution
of 10 ps. The decay prole was recorded into the computer that
is connected to the streak camera. The temperature-dependent
measurements were performed in a liquid nitrogen continuous
ow cryostat with a temperature control unit. For ISB absorp-
tion measurements, the samples were polished to a multipass
waveguide geometry with parallel 45

facets. The ISB absorp-

tion measurements were performed at RT using a Bomem MB-
100 FTIR and a cooled HgCdTe photodetector. The spectra
were obtained by taking the ratio of P-polarized spectra over
S-polarized spectra.
III. RESULTS AND DISCUSSION
The PL spectra of samples A and B have been measured
at 77 K and are shown as dashed and solid lines in Fig. 2.
Luminescence peaks of MQWs were observed at 2.268 eV
for sample A and 2.354 eV for sample B. The peak at about
2.16 eV in sample B originates from ZnCdSe cap layer while
the cap layer emission in sample A was too weak to be detected.
The PL peak moves to higher energy side for sample B is as
expected due to its decreased well width. These peak energies
are different from those in [16] due to the different well and
barrier materials composition and different well widths of the
samples used in this study. Gaussian ttings of the PL proles
give full-width at half-maximum (FWHM) as narrow as 40 and
42 meV for samples A and B, respectively. The narrow band
emission and the quantum shift (the PL peak moves to higher
energy side when well width decreases) indicate good material
quality in both samples. Shown in Fig. 3 is the QW integrated
PL intensity and PL peak energy at 77 K for samples A and B
under different excitation intensity. The solid and open squares
are the experimental data, and the solid and dotted lines are
1044 IEEE JOURNAL OF SELECTED TOPICS IN QUANTUM ELECTRONICS, VOL. 14, NO. 4, JULY/AUGUST 2008
Fig. 3. QW PL integrated intensity (open squares) and QW PL emission
energy (solid squares) at different excitation intensity for sample A (42

A well
width) and sample B (28

A well width) at 77 K.
linear ttings. No peak energy shift in the excitation intensity
range was observed, showing there is no electronic coupling be-
tween QWs, which is required for QWIP applications. In addi-
tion, linear tting of the integrated PLintensity versus excitation
intensity gives a slope less than 1, indicating free to bound transi-
tion origin of the PL emission [15]. Fig. 4 shows the normalized
PL integrated intensities of the MQWs as a function of temper-
ature for sample A (open circles) and B (solid squares). Both
samples have similar temperature-dependent behavior, showing
that the PL intensity decreases with increasing temperature due
to the increased phonon involvement at elevated temperature.
The temperature dependence of the PL intensities could be well
tted using the equation [16]
I(T) =
I
0
1 + (b
1
+ aT

)/(b
2
T
1/2
exp(E
a
/kT))
(1)
where I(T)and I
0
are the intensities at T and 0 K, and b
1
, a,
, b
2
, and E
a
are the tting parameters. The tting results are
shown as solid lines in Fig. 4. Activation energy E
a
is extracted
to be 3 and 6 meV for samples A and B, respectively.
In order to further investigate the nonradiative recombination
process of the photogenerated carriers, temperature-dependent
TRPL measurements were performed. Given in Fig. 5 are the
QW PL decay proles at 77 K for sample A (dotted line) and
sample B (dashed line). The excitation laser (solid line) is given
for reference purposes. It can be seen that all PL signals decay
exponentially with time and can be well tted by a rst-order
Fig. 4. Normalized QW PL integrated intensity at different temperatures for
sample A (open circles) and sample B (solid squares). Solid lines are the theo-
retical ttings.
Fig. 5. QW PL decay proles at 77 K for sample A (dotted line) and sample
B (dashed line). Solid line is the prole of the excitation laser.
exponential equation
I(t) = I
0
exp

PL

+ C (2)
where I (t) is the PL intensity at time t, I
0
is the PL intensity at
t = 0,
PL
is the PL decay time, and C is a constant. By tting
with the aforementioned equation, the PL decay times for both
samples at different temperatures were obtained and plotted
as a function of temperature. The results are shown in Fig. 6
by open and solid squares for samples A and B, respectively.
The PL decay time for sample B is about 440 ps at 77 K and
decreases with increasing temperature to about 120 ps at RT
due to the increased involvement of nonradiative recombination
process at elevated temperatures. On the other hand, the PL
decay time for sample A is 65 ps at 77 K and decreases to
about 25 ps at higher temperatures with the time resolution
limitation. Temperature dependences of PL decay time for both
samples could be tted using the equation that describes the
carrier lifetime as a function of temperature under assumption
of MPE capture by a defect level [16]

PL
=
1
B
m
T
1/2
exp(E
a
/kT)
(3)
where B
m
and E
a
are the tting parameters. The solid lines
shown in Fig. 6 are the tting results. Activation energy E
a
is
ZHOU et al.: INTERBAND AND INTERSUBBAND OPTICAL PROPERTIES 1045
Fig. 6. Temperature-dependent QW PL decay times for sample A (open
squares) and sample B (solid squares). Solid lines are the theoretical ttings.
obtained to be 2.85 and 5.95 meV for samples A and B, respec-
tively, and is very similar to the results obtained by the ttings of
the temperature dependences of PLintensity. These results agree
very well with our previous study [16] where the nonradiative re-
combination processes observed in ZnCdSe/ZnCdMgSe MQW
samples can be well described by hole capture by acceptor-like
defect centers through MPE that originates from lattice thermal
vibrations that cause the crossing of the carrier energy band
and the defect energy. The captured carriers will then rapidly
relax to their balanced energy position through emitting lattice
phonons. So, increasing of the temperature will cause increas-
ing of the number of phonon and further increasing of the
involvement of nonradiative process that results in decreasing
of the PL decay time and further decreasing of the PL intensity.
It is clearly seen that sample B(with narrower well) has larger
activation energy and signicantly longer PL decay times than
sample A. This indicates that there are more nonradiative defect
centers in sample A and these defect centers are most likely
from material itself instead of interface. This further indicates
better material quality of sample B than sample A.
To characterize ISB transitions of the samples, FTIR mea-
surements were performed at RT. Shown in Fig. 7 are the trans-
mittance spectra for sample A (dashed line) and sample B (solid
line). The peak absorption wavelengths were obtained at 5.35
m (0.23 eV) and 3.99 m (0.31 eV) for samples A and B, re-
spectively. For sample B, the absolute absorbance is about 75%,
and a single-pass absorbance of about 4.6%is estimated by con-
sidering the dimension of the waveguide of the sample. Fitting
the spectra with Lorentzian line shape, the FWHM (E) values
were obtained to be about 28 and 55 meV for samples A and B,
respectively. For both samples, the ratio of E/E
peak
is in the
order of 10%, which is typical for a bound-to-bound transition
and comparable to the values obtained for the well-studied III
V semiconductors [17]. In our case of MQWs with relatively
narrow QW widths, it is reasonable to assume that only the
broadening due to variations of QW width contributes apprecia-
bly to the band width of the absorption peak, and consequently,
the contribution from lifetime effects can be neglected, which
is consistent with the aforementioned results. For sample A, a
second weaker absorption peak is seen at about 2.480 m (0.5
eV) that we attribute to the bound-to-continuum absorption in
the QW region and further investigation is needed to conrm it.
Fig. 7. ISB transmittance spectra measured by FTIR for sample A (dashed
line) and sample B (solid line) (inset: multipass waveguide geometry with
parallel 45

facets for FTIR measurement).

TABLE I.
CALCULATED AND EXPERIMENTAL INTERBAND AND ISB TRANSITION
Based on envelope function approximation, assuming the
conduction and valence band offset ratio (Q
c
) of 0.8 for
ZnCdSe/ZnCdMgSe QWs [12], the energy levels of electrons
and holes in the QW region of both samples were calculated
and listed in Table I where the electrons (holes) energy posi-
tions are given relative to the minimum of QW conduction band
(valence band). The parameters used in the calculations were
from Ref. [12]. Further, interband and ISB transition energies
were deduced and also listed in the table. The bandgap values of
Zn
0.24
Cd
0.25
Mg
0.51
Se barrier and Zn
0.46
Cd
0.54
Se QW used in
the calculations were obtained from the 77 K PL emissions of
the corresponding calibrated layers, and a 70 meV downshifts
were made to get the RT value. In the table, the experimental
results of PL and FTIR are also included for easy comparison
purpose. It can be clearly seen that the experimental results agree
well with the theoretical calculations, thus conrming our pre-
vious assignments to the absorption peaks in the FTIR spectra:
the absorption peaked at 5.35 and 3.99 mm originates from ISB
transition E
1
E
2
.
IV. SUMMARY
Two n-type Zn
0.46
Cd
0.54
Se/Zn
0.24
Cd
0.25
Mg
0.51
Se MQW
structures have been grown on (0 0 1) InP substrates and their
1046 IEEE JOURNAL OF SELECTED TOPICS IN QUANTUM ELECTRONICS, VOL. 14, NO. 4, JULY/AUGUST 2008
interband and ISB properties were characterized by various op-
tical measurements. Excitation-intensity-dependent PL shows
no electronic coupling between the multiquantum wells. The
integrated PL intensities and the PL decay times of the MQWs
were measured under different temperature in the range from
77 to 290 K. Theoretical ttings of temperature dependences of
integrated PL intensities and PL decay times indicate that the
nonradiative recombination processes observed in our samples
can be well described by hole capture by acceptor-like defect
centers through MPEs. ISBabsorptions measured by FTIRwere
observed at wavelengths of 3.99 m for sample B and 5.35 m
for sample A. These mid-IR wavelengths are of great interest
for the IR photodetector applications. Theoretical calculations
based on the envelope function approximation conrmthat these
two peaks are due to the transitions from the ground state E
1
to
the rst excited state E
2
.
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Xuecong Zhou received the Ph.D. degree in physics
fromThe City College of The City University of New
York, New York, in 2005.
From 2005 to 2007, she was a Postdoctoral Re-
search Associate at the Institute for Ultrafast Spec-
troscopy and Lasers, The City College of The City
University of New York. She is currently an Applica-
tions Scientist with HORIBA Jobin Yvon, Inc., Edi-
son, NJ. She is the author or coauthor of more than
30 papers published in refereed journals. Her current
research interests include molecular beam epitaxy,
optical spectroscopy of semiconductor materials, and device applications.
Sheng-Kun Zhang received the Ph.D. degree in con-
densed matter physics fromFudan University, Shang-
hai, China, in 1999.
From 1999 to 2001, he was a Visiting Scientist at
Paul-Drude Institute. From 2001 to 2007, he was a
Research Associate at the Institute for Ultrafast Spec-
troscopy and Lasers, The City College of The City
University of New York. He is currently an Assistant
Professor of physics in the New York City College
of Technology, The City University of New York,
Brooklyn, where he is engaged in investigating quan-
tum effects of semiconductor nanomaterials and their device applications. He is
the author or coauthor of 50 publications in the eld of semiconductor materials
and devices.
Wubao Wang received the Ph.D. degree in physics
fromThe City College of The City University of New
York, in 1993.
He is currently a Senior Researcher at the Institute
for Ultrafast Spectroscopy and Lasers, The City Col-
lege of The City University of New York. His current
research interests include picosecond and femtosec-
ond time-resolved spectroscopy and lasers, ultrafast
phenomena in semiconductors, quantum-well-based
semiconductor devices, optical imaging in turbid me-
dia for medical and nonmedical applications, and
nonlinear optics. He is the author or coauthor of over 70 papers published
in referred journals, over 58 conference abstracts, and holds eight U.S. patents.
ZHOU et al.: INTERBAND AND INTERSUBBAND OPTICAL PROPERTIES 1047
Robert R. Alfano (M87SM89F01) received the
B.S. and M.S. degrees in physics fromFairleigh Dick-
inson University, Teaneck, NJ, in 1963 and 1964, re-
spectively, and the Ph.D. degree in physics from New
York University, New York, in 1972.
He is a Distinguished Professor of science and en-
gineering at The City College of The City University
of New York, New York, where he is the Director of
the Institute for Ultrafast Spectroscopy and Lasers.
His current research interests include the areas of ul-
trafast time-resolved spectroscopy, lasers, photonics,
biomedical optics, condensed matter physics, and nonlinear optics. He is the
author or coauthor of over 785 papers published and holds 102 patents. Over
the past ten years, he has received research grants from the National Science
Foundation (NSF), the National Institute of Health (NIH), the Air Force Of-
ce of Scientic Research (AFOSR), the Ofce of Naval Research (ONR), the
National Aeronautics and Space Administration (NASA), the Army Research
Ofce (ARO), and the Department of Energy (DOE).
Dr. Alfano is a Fellow of the American Physical Society (APS), the Optical
Society of American (OSA), and the New York Academy of Science.
Hong Lu received the B.S. degree in chemistry from the University of Science
and Technology, Hefei, China, and the Ph.D. degree in chemistry from The City
College of The City University of New York, New York, in 2007.
She is currently a Postdoctoral Scholar at the University of California at
Santa Barbara (UCSB), Santa Barbara. Her current research interests include
using and developing molecular beam epitaxy growth techniques for synthesis
of the materials and material structures, and characterization and processing for
fundamental understanding and device applications for the materials. She is the
author or coauthor of more than 20 papers published in refereed journals.
Maria C. Tamargo received the B.S. degree in chemistry from the University
of Puerto Rico, Rio Piedras, in 1972, and the M.S. and Ph.D. degrees in chem-
istry from The Johns Hopkins University, Baltimore, MD, in 1974 and 1978,
respectively.
From 1978 to 1984, she was a Member of the Technical Staff in AT&T
Bell Laboratories, and in Bellcore from 1984 to 1992. In 1993, she joined
The City College of The City University of New York, New York, as a Pro-
fessor of chemistry. Her current research interests include the areas of growth
and properties of semiconductor multilayered structures grown by liquid phase
epitaxy (LPE), molecular beam epitaxy (MBE), and gas source MBE, IIIV
compounds, strained-layer and short-period superlattices, surface and interface
chemistry, visible light emitters, optoelectronic devices, wide bandgap IIVI
compounds, IIVI/IIIV heteroepitaxy, low-dimensional structures, selective
area epitaxy, and mid-IR intersubband devices. She is the author or coauthor of
over 215 published papers in refereed journals and books, and holds several U.S.
patents. She has been the Chair and Co-Chair of many scientic conferences.
Prof. Tamargo is a Fellow of the American Physical Society (APS).
Aidong Shen received the B.S. degree in physics
from Xiamen University, Xiamen, China, in 1987,
and the Ph.D. degree in applied physics from Shang-
hai Institute of Optics and Fine Mechanics, Chinese
Academy of Science, Shanghai, China, in 1992.
He is currently an Assistant Professor of electrical
engineering at The City College of The City Univer-
sity of New York, New York. His current research in-
terests include semiconductor materials and devices,
particularly molecular beam epitaxial growth of III
V and IIVI semiconductors for novel photonic and
spintronic device applications. He is the author or coauthor of more than 70
articles published in refereed journals.
Prof. Shen is a member of the American Physical Society.
C. Y. Song is currently with the Institute for Microstructural Sciences, National
Research Council, Ottawa, ON, Canada.
H. C. Liu is currently with the Institute for Microstructural Sciences, National
Research Council, Ottawa, ON, Canada.