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Above-bandgap optical properties of biaxially strained GeSn alloys grown by molecularbeam epitaxyVijay Richard D’Costa, Wei Wang, Qian Zhou, Eng Soon Tok, and Yee-Chia Yeo
Citation: Applied Physics Letters 104, 022111 (2014); doi: 10.1063/1.4862659 View online: http://dx.doi.org/10.1063/1.4862659 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/104/2?ver=pdfcov Published by the AIP Publishing Articles you may be interested in Compositional dependence of optical critical point parameters in pseudomorphic GeSn alloys J. Appl. Phys. 116, 053520 (2014); 10.1063/1.4892105 Lattice constant and substitutional composition of GeSn alloys grown by molecular beam epitaxy Appl. Phys. Lett. 103, 041908 (2013); 10.1063/1.4816660 Structural and optical characterization of SixGe1x ySny alloys grown by molecular beam epitaxy Appl. Phys. Lett. 100, 141908 (2012); 10.1063/1.3701732 Investigation of the direct band gaps in Ge1xSnx alloys with strain control by photoreflectance spectroscopy Appl. Phys. Lett. 100, 102109 (2012); 10.1063/1.3692735 Increased photoluminescence of strain-reduced, high-Sn composition Ge1 x Sn x alloys grown by molecularbeam epitaxy Appl. Phys. Lett. 99, 181125 (2011); 10.1063/1.3658632
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Above-bandgap optical properties of biaxially strained GeSn alloys grownby molecular beam epitaxy
Vijay Richard D’Costa,1,a) Wei Wang,1 Qian Zhou,1 Eng Soon Tok,2 and Yee-Chia Yeo1,b)
1Department of Electrical and Computer Engineering, National University of Singapore, Singapore 1175832Department of Physics, National University of Singapore, Singapore 117551
(Received 12 November 2013; accepted 3 January 2014; published online 16 January 2014)
The complex dielectric function of biaxially strained Ge1�xSnx (0� x� 0.17) alloys grown on Ge
(100) has been determined by spectroscopic ellipsometry from 1.2 to 4.7 eV. The effect of
substitutional Sn incorporation and the epitaxial strain on the energy transitions E1, E1þD1, E00, and
E2 of GeSn alloys is investigated. Our results indicate that the strained GeSn alloys show Ge-like
electronic bandstructure with all the transitions shifted downward due to the alloying of Sn. The
strain dependence of E1 and E1þD1 transitions is explained using the deformation potential theory,
and values of �5.4 6 0.4 eV and 3.8 6 0.5 eV are obtained for the hydrostatic and shear deformation
potentials, respectively. VC 2014 AIP Publishing LLC. [http://dx.doi.org/10.1063/1.4862659]
GeSn offers exciting possibilities for bandgap and strain
engineering in the group-IV alloy system. Theory and
experiments indicate that GeSn is a direct bandgap material
for Sn composition ranging from 6 to 11%.1–4 Enhanced
absorption in the near infrared region is observed as substitu-
tional Sn is incorporated in Ge.5–7 In addition to the alloying
effect of Sn in Ge, biaxial strained GeSn epitaxially grown
on a substrate with a lower lattice constant is of great interest
for high performance complementary metal oxide semicon-
ductor devices.8–10 GeSn p-metal-oxide-semiconductor field-
effect transistors (MOSFETs) with channel mobilities higher
than Ge have been demonstrated using compressively
strained GeSn alloys.9,10 GeSn has the potential to enable
co-integration of infrared optoelectronic and electronic devi-
ces based solely on group-IV materials.
Recently, the structural and physical properties of
Ge1�xSnx (0� x� 0.145) pseudomorphically grown on Ge
(100) by molecular beam epitaxy (MBE) were reported.11
Ge1�xSnx light emitting diode with Sn content as high as 8%
was also reported.12,13 Photoluminescence has also been
observed in Ge1�xSnx (x� 0.06–0.09) quantum wells grown
on Ge.14 However, research efforts on MBE-grown GeSn
alloys have mainly focused on the indirect bandgap and the
lowest direct bandgap.2,3,15 The higher energy transitions are
also affected by composition and strain. The electronic band-
structure of biaxially strained alloys above 1 eV where the
various energy transitions E1, E1þD1, E00, and E2 are
observed at high symmetry points of the Brillouin zone16 has
not been studied experimentally. Previous reports focused on
the compositional dependence of dielectric function and
energy transitions in relaxed GeSn alloys grown by chemical
vapour deposition (CVD).4 A study on the lowest direct gap
E0 in strained Ge suggests that one may have to revisit the
deformation potentials for higher transitions in Ge.17
Deformation potentials for E0 in GeSn (Ref. 15) are known,
but no data are available for transitions above E0. The deter-
mination of E1, E1þD1, E00, and E2 in strained Ge-rich
GeSn alloys will allow us to gain insight into deformation
potentials which are important for predicting the energy
shifts resulting from strain.
In this Letter, we report the dielectric function and the
above-bandgap electronic transitions of strained GeSn alloys
grown using MBE. Spectroscopic ellipsometry was used to
obtain the complex dielectric function of the alloys. The
dielectric function of the material contains sharp features
which are related to E1, E1þD1, E00, and E2 in the joint den-
sity of states in the electronic bandstructure of the material.
The compositional dependence of E1, E1þD1, E00, and E2 is
determined using a critical point analysis.18 The determina-
tion of dielectric function will not only elucidate the elec-
tronic bandstructure of strained GeSn alloys but will also
enable accurate process metrology for the fabrication of opti-
cal and electronic devices.
Crystalline Ge1�xSnx (0� x� 0.17) were grown directly
on Ge (100) substrates in a solid-source MBE system at the
National University of Singapore (NUS) with a base pressure
of 3� 10�10 Torr. The substrates were 4 in. diameter,
single-side polished, and As-doped with a doping level of
1� 1017 cm�3. The Ge wafer was cleaned using a diluted
hydrofluoric (DHF) etch and loaded immediately into the
load-lock chamber. The wafer was pre-heated to 630 �C to
remove the germanium oxide. The substrate temperature was
adjusted to between 100 �C and 170 �C to enable growth of
high quality Ge1�xSnx films with thicknesses ranging from
200 nm to 25 nm as x varied from 0.02 to 0.17. The alloy
composition was tuned by varying Ge and Sn fluxes.
The samples were investigated for their crystalline qual-
ity, composition, strain, and thickness by high-resolution X-
ray diffractometry (HR-XRD) at Singapore Synchrotron
Light Source (SSLS). Figure 1(a) shows the x-2h curves for
three GeSn alloys. The peak at lower 2h angle in each (004)
scan corresponds to GeSn alloys, and it shifts to a lower
angle with increasing Sn composition, indicating incorpora-
tion of Sn in the Ge lattice. We determined the GeSn thick-
nesses from the Pendellosung fringes which are observed
in all our samples, indicating coherent epitaxial films.11
The thicknesses were also independently confirmed by
a)Electronic mail: [email protected])Electronic mail: [email protected]
0003-6951/2014/104(2)/022111/4/$30.00 VC 2014 AIP Publishing LLC104, 022111-1
APPLIED PHYSICS LETTERS 104, 022111 (2014)
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cross-sectional transmission electron microscopy (XTEM).
(115) reciprocal space mapping (RSM) for a representative
sample is shown in Figure 1(b) from which the in-plane
strain ek and the Sn composition are determined.11,19 Both
Ge and GeSn peaks have the same value of reciprocal lattice
vector along [110] Qk, indicating that the epitaxial GeSn
layer is fully strained to Ge. As previously reported for
strained Ge1�xSnx alloys,11 the critical thickness to obtain
high quality or pseudomorphic alloys decreases as a function
of x. Ge0.83Sn0.17 alloy, which is also the thinnest film,
appears to have larger full-width at half-maximum (FWHM)
compared to the thicker alloys with lower Sn content. Using
Scherer’s formula, we verified that the FWHM in (004)
curves is mainly due to the finite thickness of our films and
not caused by the presence of non-uniformities and defects.11
Figure 1(c) shows an XTEM image for the Ge0.98Sn0.02
alloy, indicating that the film is of uniform thickness with a
sharp interface between the film and the substrate. High
magnification XTEM images for Ge0.98Sn0.02, Ge0.92Sn0.08,
and Ge0.83Sn0.17 alloys are shown in Figures 1(d)–1(f),
respectively. In addition, atomic force microscopy (AFM)
showed that the root mean square (RMS) roughness of
Ge0.92Sn0.08 alloy is less than 1 nm (not shown here).
Spectroscopic ellipsometry measurements were carried
out at room temperature using a rotating analyzer ellipsome-
ter manufactured by J. A. Woollam Co.20 The ellipsometric
angles Psi and Delta were acquired at 10 meV energy steps
for angles of incidence 65� and 75� from 1.2 to 4.7 eV. A ref-
erence Ge film grown on Ge substrate was characterized
along with the GeSn alloys. The samples were modeled as a
three-layer system containing a Ge substrate, the GeSn film,
and a surface layer. The surface layer was modeled as a
GeO2 layer.21 The Ge substrate used in growth experiments
was characterized separately, and the dielectric function
obtained was used in tabulated form in the model. The com-
plex dielectric function of GeSn film is modeled using a dis-
persion model as developed by Herzinger and Johs following
the theoretical work of Kim and Garland.22,23 The model
takes into account the full analytic form of joint density of
states and is thus capable of describing the measured dielec-
tric function very accurately. Four parametric oscillators are
needed to describe the four critical point transitions E1,
E1þD1, E00, and E2 which are observed in the measured
data range. The data are processed using the procedure fol-
lowed in Ref. 4 which gives us the non-parametric or point--
by-point fit dielectric function in addition to the
parametrized dielectric function. The agreement between the
two is excellent confirming the Kramers-Kronig consistency
of the non-parametric function. It is to be noted here that an
isotropic dispersion model fully accounts for the observed
dielectric response of strained GeSn alloys although aniso-
tropic optical response is expected under the influence of
biaxial strain. This behavior is also observed in other
strained systems including Si and SiGe and is expected as
the acquired spectroscopic ellipsometry data correspond to
the in-plane component of dielectric function for the experi-
mental conditions used.24–26 Figure 2 shows the dielectric
function of GeSn alloys. The dielectric function of strained
GeSn alloys is very similar to Ge and shifts to the left with
respect to Ge with increasing Sn concentration, indicating
the alloying effect of Sn on the electronic bandstructure of
pure Ge.4
The parameterized dielectric function obtained for the
strained alloys is very useful for monitoring film thickness
and composition during device fabrication. For critical point
analysis, the non-parametric dielectric function is preferred to
the parameterized dielectric function.4 The non-parametric
dielectric function is numerically differentiated twice using
17 Savitzky-Golay coefficients corresponding to a polynomial
of order 5. We ensured that the number of smoothing coeffi-
cients used did not distort the line shape. The derivatives of
the experimental dielectric function were fitted using4
d2edE2¼X
j
AjeiUj
½E� Ej þ iCj�2; (1)
where Aj is the amplitude for transition j, Uj is the phase
angle, Ej is the critical point energy, and Cj is the broadening
FIG. 1. HRXRD results, showing (a) (004) x–2h scans of selected GeSn
alloys, (b) (115) RSM of a Ge0.83Sn0.17 alloy. Qk and Q? are the reciprocal
vectors along [110] and [001] and are expressed in reciprocal lattice units
(rlu). The wavelength of X-ray radiation used was 1.538 A. (c) Low magnifi-
cation XTEM image for a Ge0.98Sn0.02 alloy. High magnification XTEM
images showing the interface between Ge1�xSnx and Ge, (d) x¼ 0.02, (e)
x¼ 0.085, and (f) x¼ 0.17. The virtually defect-free interface indicates the
good crystalline quality of GeSn epitaxially grown on Ge.
FIG. 2. (a) Real and (b) imaginary parts of the complex dielectric function
of selected strained Ge1�xSnx alloys and a relaxed Ge film. The legend
applies to both plots.
022111-2 D’Costa et al. Appl. Phys. Lett. 104, 022111 (2014)
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parameter. The summation covers all the four transitions E1,
E1þD1, E00, and E2. The imaginary and real parts of the
dielectric function are fitted simultaneously by a least-square
procedure which follows the Levenberg-Marquardt algo-
rithm.27 The procedure was first verified on a reference Ge
film grown on a Ge substrate. The critical point parameters
for this film were found to be in excellent agreement with
the bulk Ge values reflecting the accuracy of our procedure
as well as the quality of our Ge film.18 The critical point
analysis of a GeSn alloy is shown in Figure 3. The sharp fea-
tures in the derivative spectra correspond to E1, E1þD1, E00,
and E2 which are extracted from a fit using Eq. (1).
The compositional dependence of energy transitions in
the strained GeSn alloys is shown in Figure 4. E1, E1þD1,
E00, and E2 reduce with Sn composition but are elevated with
respect to relaxed GeSn alloys. E1þD1 shows larger devia-
tion between the experimental values and the relaxed values
compared to E1. Besides the alloying effect of Sn, the pres-
ence of biaxial strain will influence the critical point energy
values. We use the deformation potential theory to under-
stand the effect of strain on energy transitions.28,29 In this pa-
per, we focus on E1 and E1þD1. Strain analysis is not
established for E00 and E2 in Ge and SiGe. The deformation
potentials of E00 and E2 are not well studied, perhaps due to
an incomplete understanding of their origin.4,30 The expres-
sions for E1 and E1þD1 in GeSn alloys can be written as
E1ðx; eÞ ¼ E1ðxÞ þ D1ðxÞ=2þ EH �ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiES
2 þ ðD1ðxÞ=2Þ2q
;
(2)
ðE1 þ D1Þðx; eÞ ¼ ðE1 þ D1ÞðxÞ � D1ðxÞ=2þ EH
þffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiES
2 þ ðD1ðxÞ=2Þ2q
; (3)
where EH ¼ ð2=ffiffiffi3pÞD1
1 1� c12=c11ð Þek gives the energy shift
due to the hydrostatic component of the strain and ES ¼�
ffiffiffiffiffiffiffiffiffiffið2=3
pÞD3
3ð1þ 2c12=c11Þek is the energy shift due to the
shear component of the strain. Linear interpolation between
Ge and a-Sn is used for the elastic constant ratio c12/c11.31
D11 and D3
3 are the hydrostatic deformation and shear defor-
mation potentials, respectively. The deformation potentials
for Ge are taken from Ref. 30 whereas experimental values
for a-Sn are not available yet. The compositional depend-
ence for E1(x), (E1þD1)(x), and D1ðxÞ is taken from Ref. 4.
Equations (2) and (3) indicate that the EH and
ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiES
2 þ ðD1ðxÞ=2Þ2q
tend to cancel each other for E1 whereas
they both add up for E1þD1. This qualitatively explains the
observed behavior of E1 and E1þD1 in our strained alloys
and is analogous to what is found in strained SiGe alloys.26
Figure 5(a) shows that the theory (dotted line) using Ge de-
formation potentials accounts for observed E1 (triangles) but
overestimates E1þD1 (circles). It is quite possible that the
discrepancy between experiment and theory is caused by the
use of Ge deformation potentials for E1 and E1þD1. This is
not surprising because even the deformation potentials for
the widely studied E0 gap in Ge vary significantly in litera-
ture.17 It may be pointed out here that both the deformation
potentials for SiGe had to be adjusted to explain the strain
dependence of E1 and E1þD1.26 We analyze the average of
E1 and E1þD1 which contains only D11. Adding Eqs. (2) and
(3) and calling the average of the two transitions as �E1, we
obtain ( �E1(x,e) � �E1(x))¼DE¼EH as the energy shift due to
strain. We plot DE as a function of in-plane component of
strain in Figure 5(b). The dotted curve is the simulation of
experimental data using the Ge value for D11. It clearly shows
the discrepancy between experimental and theoretical
expression as observed for E1þD1. We model the experi-
mental data with D11 as a fitting parameter and obtain a value
of �5.4 6 0.4 eV. Figure 5(a) shows the resulting theoretical
curve (solid line) which is in very good agreement with the
FIG. 3. Numerical second derivatives of (a) real and (b) imaginary parts of
the dielectric function of a Ge0.92Sn0.08 alloy. Experimental data are plotted
in circles, and the model is plotted using solid lines.
FIG. 4. Compositional dependence of (a) E1 and E1þD1 (b) E00 and E2 in
strained Ge1�xSnx alloys, plotted using square symbols. The solid curves
represent the compositional dependence of transition energies for the relaxed
alloys taken from Ref. 4.
FIG. 5. (a) Strain analysis of E1 (triangles), �E1 (squares), and E1þD1
(circles). The dotted curve represents calculated energy using the Ge value
of �8.6 eV for D11. The solid curve represents calculated energy using the
new D11 value of �5.4 eV for GeSn. (b) Energy shift DE for �E1 plotted as a
function of in-plane strain. The dotted curve represents the energy shift cal-
culated using the Ge value for D11. The solid line is a fit with DE¼D1
1f ðekÞ,where f ðekÞ ¼ ð2=
ffiffiffi3pÞ 1� c12=c11ð Þek.
022111-3 D’Costa et al. Appl. Phys. Lett. 104, 022111 (2014)
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experimental data for �E1 (squares). Note that D11 for GeSn
lies between pure Ge (�8.6 eV) and the theoretical value of
a-Sn (�3.8 eV), indicating that it is consistent with the
expected trend for D11.32 Eliminating the hydrostatic potential
from Eqs. (1) and (2), we obtain a value of 3.8 6 0.5 eV for
D33 of GeSn. Using the new values of D1
1 and D33, we
re-calculate the strain correction for E1þD1, which now
shows excellent agreement with the experimental data. E1
now overlaps with the theoretical curve calculated using the
Ge deformation potentials. It appears that the discrepancy
between experimental data and theory was primarily caused
by the use of Ge values to account for the strain effects in
GeSn. Our strain analysis for Ge-rich GeSn alloys indicates
that values of �5.4 eV and 3.8 eV for D11 and D3
3, respec-
tively, are required to account for the energy shifts caused by
strain in E1 and E1þD1.
In conclusion, we have determined the dielectric function
of biaxially strained GeSn alloys which indicate that the alloys
obey Ge-like bandstructure. The compositional dependence of
E1, E1þD1, E00, and E2 was determined using a critical point
analysis and interpreted in terms of the relaxed alloys. The de-
pendence of E1 and E1þD1 on strain was explained using the
deformation potential theory. We propose that a hydrostatic
potential value of �5.4 eV and a shear deformation potential
value of 3.8 eV can be used to calculate the energy shifts for
E1 and E1þD1 in strained GeSn alloys.
This work was supported by the National Research
Foundation under the Competitive Research Programme
(Grant No. NRF-CRP6-2010-4).
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