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APPLIED PHYSICS LETTERS 88, 112111 共2006兲

Ultrafast recombination in Si-doped InN


Ricardo Ascázubi and Ingrid Wilkea兲
Department of Physics, Applied Physics and Astronomy, Rensselaer Polytechnic Institute, Troy,
New York 12180
Shinho Cho
Department of Photonics, Silla University, Busan, Republic of Korea
Hai Lu and William J. Schaff
Department of Electrical and Computer Engineering, Cornell University, Ithaca, New York 14853
共Received 12 December 2005; accepted 17 February 2006; published online 16 March 2006兲
We report femtosecond near-infrared transient photoreflection measurements of native n-type
indium nitride and silicon-doped indium nitride thin films. The overall time dependence of the
ultrafast reflectivity transient is characterized by the different time scales of carrier cooling and
carrier recombination. Experimental analysis demonstrates nonradiative recombination in the
picosecond and subpicosecond range as the dominant recombination mechanism at room
temperature even at very high carrier concentrations. Silicon-doped InN films exhibit carrier
lifetimes as short as 680 fs. © 2006 American Institute of Physics. 关DOI: 10.1063/1.2185407兴

InN is regarded as an essential component of the group In this letter we present a study of carrier dynamics in
III-nitride semiconductor system. Recent progress towards InN thin films by femtosecond time-resolved reflectivity
the growth of high quality InN thin films has led to the measurements. Our InN thin films are grown9 by molecular
revision of the fundamental band gap of InN1 from 2.0 to beam epitaxy 共MBE兲 on c-plane sapphire with AlN nucle-
0.69 eV. This discovery currently stimulates research on the ation layers and GaN buffer layers. Unintentionally doped
fundamental optical and electronic properties of InN and the InN films used in this work have a sheet carrier concentration
development of applications in many optoelectronic devices ranging from 7 ⫻ 1017 to 1 ⫻ 1019 cm−3 and silicon-doped
and systems. It has been demonstrated2 that InN is an effi- InN films have a carrier concentration ranging from
cient emitter of broadband THz radiation for time-domain 2 ⫻ 1019 to 4 ⫻ 1020 cm−3. The film thickness ranges from
THz sensing and imaging. In1−xGaxN also has a strong po- 150 nm to 4.6 ␮m and the mobility of these samples ranges
tential for the fabrication of efficient solar cells.3 Addition- from 80 to 1673 cm2 / V s. Transient photoreflection has been
ally, InN is of interest for photovoltaic devices in space ap- investigated with an optical pump-probe arrangement. The
plications, because it exhibits a very high radiation InN samples are excited with 130 fs Ti: S laser pulses with a
resistance.3 In order to materialize the potential of InN for wavelength centered at 800 nm. The maximum excitation la-
device applications the understanding of carrier dynamics, in ser power is 400 mW and the laser pulse repetition rate is
particular of phonon scattering and carrier recombination, is 82 MHz. The pump and probe beams are focused by a lens
crucial. 共f = 200 mm兲 on the InN sample. A 10 ␮m pinhole was used
Due to the polar character of InN, optical phonons are to achieve spatial overlap of the pump and probe beams and
expected to play a significant role in the carrier scattering to estimate the focal spot size. The estimated optically gen-
process. Chen et al.4 studied hot carrier relaxation in InN by erated carrier density is 1.4⫻ 1020 cm−3. All samples have
time-resolved photoluminescence measurements. They ob- been studied at room temperature.
served that hot carriers are fully relaxed after 10 ps. High The polarization of the pump beam is parallel to the
speed I-V characterization5 has shown, through power bal- plane of incidence and perpendicular to the probe beam po-
ance considerations, that the LO-phonon scattering time in larization. In order to study the dependence of the photore-
InN should be around 200 fs, while Raman spectroscopy6 flection signal with optical pump power a variable neutral
indicates a LO-phonon lifetime of 0.7– 1.3 ps through uncer- density filter was used. Modulation and lock-in detection has
tainty principle considerations. These values of the LO- been used to observe reflectivity variations 共⌬R / R兲 of 10−5.
phonon scattering time are far from those predicted by The transient reflectivity of an optically excited semi-
theory,7 which range from 16 to 31 fs. conductor is explained by a variation of the complex refrac-
Furthermore, it has been reported8 that carrier recombi- tive index through several effects like the absorption change
nation at 20 K is dominated by radiative recombination with due to band filling 共BF兲, band-gap renormalization 共BGR兲,
nanosecond carrier lifetimes. In contrast, recombination at free carrier absorption, and carrier recombination. Our inter-
room temperature is dominated by nonradiative recombina- pretation of the temporal evolution of the transient reflectiv-
tion. It has also been observed that the nonradiative recom- ity of InN follows the calculations of band-gap renormaliza-
bination lifetime depends inversely on the carrier concentra- tion and band filling as outlined.10 In our picture the carriers
tion and assumes ⬃50 ps at n ⬇ 1019 cm−3.8 Localized acquire a hot, thermalized energy distribution during excita-
nonradiative recombination centers are presumed to be re- tion itself and then cool via phonon emission. This assump-
sponsible for carrier trapping. tion is based on the fact that we perform our measurements
at high excitation densities that favor quick thermalization of
a兲
Electronic mail: wilkei@rpi.edu the hot carriers via carrier-carrier scattering and the experi-

0003-6951/2006/88共11兲/112111/3/$23.00 88, 112111-1 © 2006 American Institute of Physics


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112111-2 Ascázubi et al. Appl. Phys. Lett. 88, 112111 共2006兲

FIG. 1. Recorded reflectivity transient for a silicon-doped InN film. 共n FIG. 2. Recombination lifetimes vs carrier concentration. Silicon-doped InN
= 1020 cm−3, ⌬nopt = 1.4⫻ 1020 cm−3.兲 The reflectivity decay is fitted by a samples show recombination lifetimes lower by an order of magnitude than
single exponential 关exp共−t / ␶兲兴 with ␶ = 1.19 ps. This process is attributed to the undoped counterparts. The carrier concentration was determined by dc
nonradiative defect-related recombination. The inset shows the reflectivity Hall measurements.
transient for an undoped InN film 共n = 7 ⫻ 1018 cm−3, ⌬nopt = 1.4
⫻ 1020 cm−3兲. Two processes are observed therein: carrier cooling within the
first 2 – 3 ps and nonradiative recombination at later times. lifetimes by an order of magnitude lower than the uninten-
tionally doped InN samples. The carrier lifetime exhibits an
inverse dependence on the carrier concentration for carrier
mental observation that InN exhibits rather long LO-phonon concentrations up to 4 ⫻ 1020 cm−3. The reduction of the re-
scattering times 共⬃200 fs兲.5 Photoreflection transients of un- combination lifetime in silicon-doped InN compared to un-
intentionally doped InN and InN: Si are shown in Fig. 1. For doped InN suggests that silicon impurities may act as ul-
our samples, the temporal evolution of the reflectivity signal trafast trapping and recombination centers in InN. Our
is characterized by an initial fast decrease, followed by a observation of an inverse relationship between carrier life-
quick rise and a second much slower decay of the reflectiv- time and carrier concentration in InN agree with previous
ity. In the Fig. 1 inset, the reflectivity change within the first time-resolved differential transmission measurements of un-
2 – 3 ps of our measurements reflects the carrier cooling. The doped InN.12 However, our time-resolved reflectivity mea-
temporal shape of the reflectivity is dominated by the inter- surements result in carrier lifetimes that are shorter by an
play of band-gap renormalization and band filling. At short order of magnitude. It is noteworthy that reflection experi-
delays and high carrier temperature band filling is far from ments probe the InN surface up to the optical penetration
saturation and the BGR effect, which is strong in InN,11 depth 共200 nm at 800 nm wavelength1兲 as opposed to trans-
dominates the reflectivity signal. This results in a decrease in mission experiments where the bulk and the surface are
reflectivity. As carriers cool and relax towards the band edge probed. InN exhibits a high surface charge accumulation
the change in absorption due to BF gets larger than the arising from surface defects. This high defect density near
change due to BGR. This leads to an increase of the reflec- the surface may be responsible for the difference between
tivity. The subsequently observed slow decay of the reflec- reflection and transmission carrier lifetimes.
tivity is attributed to carrier trapping and recombination. The In order to investigate the nature of the carrier recombi-
carrier recombination lifetime was obtained from these mea- nation process reflectivity transients have been measured for
surements by fitting a single exponential to the reflectivity various excitation fluences. The observed peak signal ampli-
decay. The carrier lifetimes in dependence of carrier concen- tude versus fluence as well as the carrier lifetime versus flu-
trations are illustrated in Fig. 2. They range from 64 ps for a ence are shown in Fig. 3. The reflectivity exhibits a linear
carrier concentration of n = 7 ⫻ 1017 cm−3 to a carrier lifetime dependence on fluence. This is in agreement with intraband
of 680 fs at n = 4 ⫻ 1020 cm−3. The overall temporal shape of free carrier absorption. According to the Shockley-Read-Hall
the reflectivity transient is characterized by the different time theory12 the carrier lifetime ␶ is expected to be independent
scales of carrier cooling and carrier recombination. For rela- of the total carrier density n + ⌬n if nonradiative recombina-
tively long carrier lifetimes the carrier cooling effect is tion is the dominant mechanism among nonradiative
clearly visible in the reflectivity transient as indicated by the 关␶nr = 1 / 共Ndef␴defv兲, radiative 共␶rad = Brad / 共n + ⌬n兲兴 and Auger
initial reflectivity decrease and the broad reflectivity peak recombination 关tA = CAuger / 共n + ⌬n兲2兴:
共Fig. 1, inset兲. For short carrier lifetimes the broad reflectiv-
ity peak vanishes 共Fig. 1兲. Although we are not able to de- 1 1 n + ⌬n 共n + ⌬n兲2
duce quantitatively the LO-phonon scattering rate from these = + + . 共1兲
␶ ␶nr Brad CAuger
measurements, our observation of the overall temporal shape
of the reflectivity transient supports that the LO-phonon scat- The carrier lifetime ␶ observed in our experiments is
tering time in InN is significantly longer than the 31 fs pre- independent of fluence within the error of our measurements.
dicted by theory. Therefore, we conclude that nonradiative carrier recombina-
Next, we discuss the carrier lifetime. Our results demon- tion is the dominant recombination mechanism for carrier
strate that silicon-doped InN samples have recombination densities up to n ⬇ 1020 cm−3 at room temperature. Radiative
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112111-3 Ascázubi et al. Appl. Phys. Lett. 88, 112111 共2006兲

ultrafast application such as an Auston switch.13 InN is espe-


cially attractive for those applications because of the absence
of low side valleys14 in this material and because the band
gap of InN is lower than that of other ultrafast photoconduc-
tive materials such as LT-GaAs. This may enable the use of
InN THz detectors with solid-state 1.55 ␮m fiber lasers in
portable THz spectroscopy systems.
This material is based upon work supported by the
National Science Foundation under Grant No. 0333314.
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