Generation and Detection of Ultrabroadband Terahertz Radiation Using Photoconductive Emitters and Receivers

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Generation and detection of ultrabroadband terahertz radiation using

photoconductive emitters and receivers


Y. C. Shen, P. C. Upadhya, H. E. Beere, E. H. Linfield, A. G. Davies et al.

Citation: Appl. Phys. Lett. 85, 164 (2004); doi: 10.1063/1.1768313


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APPLIED PHYSICS LETTERS VOLUME 85, NUMBER 2 12 JULY 2004

Generation and detection of ultrabroadband terahertz radiation using


photoconductive emitters and receivers
Y. C. Shen, P. C. Upadhya, H. E. Beere, and E. H. Linfielda)
Cavendish Laboratory, University of Cambridge, Madingley Road, Cambridge CB3 0HE, United Kingdom
A. G. Davies
School of Electronic and Electrical Engineering, University of Leeds, Leeds LS2 9JT, United Kingdom
I. S. Gregory, C. Baker, W. R. Tribe, and M. J. Evans
TeraView Ltd., Unit 302/304 Cambridge Science Park, Milton Road, Cambridge, CB4 0WG United
Kingdom
(Received 3 February 2004; accepted 10 May 2004)
We report the coherent generation and detection of ultrabroadband terahertz (THz) radiation using
low-temperature-grown GaAs photoconductive antennas as both emitters and receivers. THz
radiation with frequency components over 15 THz was obtained, the highest reported for a THz
time-domain system based on photoconductive antennas. Such a system has a smooth spectral
distribution between 0.3 and 7.5 THz, ideal for spectroscopic applications. In addition, sharp
spectral features at 8.0 and 8.8 THz were observed, and explained in terms of optical phonon
resonances in the photoconductive antennas. © 2004 American Institute of Physics.
[DOI: 10.1063/1.1768313]

The coherent generation and detection of terahertz 共THz兲 tions in the GaAs antennas are directly observed with a high
radiation using ultrashort optical pulses has been investigated time resolution, with the frequency and decay time of the
intensively during the last decade. The pulse width of com- coherent oscillations being determined by fitting the experi-
mercially available mode-locked Ti:sapphire lasers is ap- mental results with an exponentially decaying sine wave.
proaching 10 fs and, with such ultrashort laser pulses, the The general experimental arrangement for coherent gen-
spectral distribution of the detected THz radiation has been eration and detection of ultrabroadband THz radiation has
reported to be over 30 THz, using thin electro-optic (EO) been described previously.8 In brief, a Ti:sapphire laser pro-
crystals as the emitter and detector.1,2 In contrast, the spectral vides visible/near-infrared pulses of 15 fs duration at a center
bandwidth of THz time-domain spectroscopy systems3 em- wavelength of 790 nm with a repetition rate of 76 MHz. The
ploying photoconductive 共PC兲 antennas, the main alternative output is split into two parts: a 400 mW beam is focused
for generating and detecting coherent THz radiation, has onto the surface of a biased LT-GaAs PC emitter for THz
been limited to ⬃3 THz.4,5 This limited bandwidth of PC generation, and a 30 mW beam serves as the probe beam to
antennas was originally explained by either the finite carrier gate the PC receiver antenna for THz detection. The PC
lifetime or the momentum relaxation time of the carriers in emitter has a gap of 400 ␮m, and is biased using an 11 kHz
the substrate. However, low-temperature-grown GaAs 共LT- chopped sinusoidal wave with peak amplitude ±120 V. For
GaAs兲 PC antennas have recently been used to detect ultra- both PC emitter and receiver, the NiCr/ Au electrodes
broadband (over 30 THz) electromagnetic radiation gener- (Ti/ Pd/ Au for receiver) are vacuum-evaporated on a 1.0-
ated by optical rectification of ultrashort laser pulses in thin ␮m-thick LT-GaAs layer grown at 220 º C on a
EO crystals.6,7 The fast response of the PC receivers was 0.53-mm-thick semi-insulating GaAs substrate. Ex situ post-
explained by the fast rise time of the photogenerated carrier growth annealing of the LT-GaAs (see Ref. 9) allowed opti-
concentration, which is determined by the laser pulse width.6 mization of the carrier lifetimes and resistivities for the indi-
vidual PC receiver and emitter. Specifically, the carrier
Very recently we also observed ultrabroadband (over
lifetimes for the receiver and emitter are 0.1 and 10 ps, re-
30 THz) THz emission from LT-GaAs PC antennas, using a
spectively, as determined from transient reflectance
20-␮m-thick ZnTe crystal as the THz sensor.8 Pronounced
measurements.9 The laser pulse width incident on the PC
THz emission, originating from optical phonon oscillations
emitter and receiver is estimated to be 20 fs.
in GaAs 共␯TO ⬅ 8.02 THz; ␯LO ⬅ 8.76 THz兲 was also ob-
The emitted THz pulse is collimated and focused onto
served, and the shape of the measured THz signal was fur-
the sample by a pair of parabolic mirrors. The transmitted
ther complicated by the phonon resonances of the ZnTe de-
THz pulse is then collected and focused using another pair of
tector 共␯TO ⬅ 5.3 THz; ␯LO ⬅ 6.2 THz兲.
parabolic mirrors onto the surface of a LT-GaAs antenna for
In this letter, we report the first system combining a PC PC detection. It should be noted that the geometry used for
antenna emitter and a PC antenna receiver for the generation PC generation and detection is critical. Following the tech-
and electric-field-resolved detection of ultrabroadband THz nique in Ref. 8, the THz radiation generated in the PC emit-
radiation. The measured THz signal has a smooth spectral ter is collected in a reflection geometry [see Fig. 1(a)],
distribution from 0.3 to 7.5 THz, ideal for spectroscopic ap- thereby avoiding absorption and dispersion in the GaAs sub-
plications. Furthermore, the coherent optical phonon oscilla- strate. This is essential for observing the high frequency
components of the generated THz radiation. Another advan-
a)
Electronic mail: eh110@cam.ac.uk tage of such a configuration is that the back of the GaAs

0003-6951/2004/85(2)/164/3/$22.00 164 © 2004 American Institute of Physics


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Appl. Phys. Lett., Vol. 85, No. 2, 12 July 2004 Shen et al. 165

FIG. 2. Measured (points) and calculated (curve) temporal THz waveform


between 1.0– 4.0 ps. Note that the phonon oscillations can be seen immedi-
ately after the initial transient [see Fig. 1(a)], and extend over 12.0 ps, al-
though for clarity, only a restricted interval is shown here.

Ultrabroadband PC detection was first demonstrated by


Kono et al.6 using, for THz generation, optical rectification
of a femtosecond laser pulse in a 100-␮m-thick ZnTe crystal
(i.e., EO generation and PC detection). The amplitude of the
THz electric field measured in our work is about two orders
FIG. 1. (a) Temporal THz waveform and, (b) its corresponding Fourier
transform amplitude spectrum. The arrows mark spectral features corre-
of magnitude larger (four orders of magnitude larger in THz
sponding to TO and LO (phonons of the GaAs vTO ⬅ 8.02 THz; vLO power) than that reported by Kono et al.,6 owing to the larger
⬅ 8.76 THz) crystal. Inset of (a) shows the schematic geometry of the bi- power available from the PC emitter. Therefore, the combi-
ased and asymmetrically excited LT-GaAs PC emitter (antenna gap of nation of a PC emitter and a PC receiver antenna proves an
400 ␮m); (b) shows the schematic geometry of an LT-GaAs PC receiver ideal THz system for practical spectroscopy applications. As
(blunted bowtie antenna: 8 ␮m gap, 90° bow angle, 8 ␮m length).
an example, Fig. 3 shows the vibrational spectrum of maltose
measured with such a system. Samples were prepared by
substrate is free to be modified to minimize THz reflections mixing finely milled maltose polycrystalline powder (Sigma
(and thus increase the spectral resolution of the obtained THz Aldrich Co.) with polyethylene powder (Sigma Aldrich Co.)
spectra), or for cooling schemes5 to be added. THz detection in a mass ratio of 1:10, and then compressing the mixture to
form a pellet of thickness 1.3 mm. The low frequency vibra-
was achieved using the geometry shown in Fig. 1(b), with
tional modes of maltose were previously measured with a
once again absorption and dispersion in the GaAs substrate
conventional THz time-domain spectrometer, but the fre-
minimized. In all measurements, the variable delay stage,
quency range was limited to 0.3− 3.0 THz.10 In contrast, here
which provides the time delay between the THz pulse and we resolved 14 vibrational modes over a much wider fre-
the probe pulse, is scanned over a distance of 2 mm, provid- quency range 共0.3– 7.3 THz兲, demonstrating the extended
ing a spectral resolution of 75 GHz 共2.5 cm-1兲. The whole bandwidth of this THz spectroscopy system. Note, that these
apparatus is enclosed in a vacuum-tight box, which is purged
with dry nitrogen gas to reduce the effects of water vapor
absorption. Measurements are performed at room tempera-
ture.
Figure 1(a) shows a typical temporal THz waveform
generated from the PC emitter and detected with the PC
receiver, with Fig. 1(b) showing the corresponding frequency
spectrum. In the frequency domain, the spectrum of the THz
radiation extends continuously to over 15 THz, except for a
spectral dip at 8 THz and a distinct peak at 8.7 THz. These
two spectral features are explained as originating from
longitudinal-optical (LO) and transverse-optical (TO) pho-
non resonances in the GaAs PC antennas. In the time do-
main, the phonon oscillations can be seen immediately after
the initial transient, and extend over 12 ps. These oscillations
were fitted with an exponentially-decaying sine wave:
FIG. 3. Fourier-transform amplitude spectrum of the THz radiation mea-
ETHz共t兲 = C1e−t/␶ sin 共2␲␯t − C2兲. As shown in Fig. 2, the sured after transmitting through a pure polyethylene reference pellet (upper
agreement between the fitted and the measured THz signal is trace), and a maltose/polyethylene sample pellet (lower trace). Arrows indi-
very good. The best-fit results give an oscillating frequency cate vibrational modes of maltose at frequencies of 1.11, 1.61, 2.0, 2.21,
2.39, 2.64, 2.93, 3.33, 3.6, 4.28, 4.61, 5.07, 6.35, and 7.0 THz. Note that the
v = 8.7 THz and a decay time ␶ = 3 ps, confirming that these Fourier transforms were performed using the first derivatives of the mea-
oscillations originate from LO phonon resonances in the sured signals, to minimize the possible spectral artefacts caused by an offset
GaAs 共␯LO ⬅ 8.76 THz兲. in the measured signals. Inset shows the molecular structure of maltose.
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166 Appl. Phys. Lett., Vol. 85, No. 2, 12 July 2004 Shen et al.

observed vibrational modes correspond to both inter- and peak amplitude of THz signal to the noise level) than
intra-molecular interactions.11 EO-detection,8 up to frequencies in excess of 8 THz.
In a previous study,8 we used EO detection with a 20- In conclusion, we have used LT-GaAs antennas for both
␮m-thick ZnTe crystal to study THz radiation from a similar generating and detecting ultrabroadband THz radiation. Our
LT-GaAs antenna (PC-generation and EO detection). The results show that such a PC-generation/PC-detection scheme
measured THz signals, however, were far more complicated, leads to a smooth spectral distribution up to 8 THz and pro-
with two additional spectral features at 5.3 and 6.2 THz. It is vides better signal-to-noise-ratio, compared with both EO-
clear that these two additional spectral features were caused generation/PC-detection6 and PC-generation/EO-detection8
by the ZnTe detector 共␯TO ⬅ 5.3 THz; ␯LO ⬅ 6.2 THz兲 used schemes. It thus makes an ideal system for THz time-domain
in previous studies. On the other hand, the THz signals mea- spectroscopy in the frequency range 0.3− 7.5 THz.
sured in the previous study8 covered a broader (over 30 THz)
spectral range. The reduced spectral coverage in the present This work was supported by the Research Council UK
study is mainly a result of the decreased sensitivity of the PC (Basic Technology Programme), Toshiba Research Europe
antennas at high frequencies. For the EO detection employed Ltd. (E.H.L.), and the Association of Commonwealth Uni-
in Ref. 8, the EO crystal detects the polarization change of versities (P.C.U.). I.S.G. and C.B. thank EPSRC for student-
the probe beam induced by the THz electric field in the sen- ship.
sor crystal. Therefore, the detected signal is simply propor-
tional to the THz electric field. For PC detection of ultra- 1
P. Y. Han and X.-C. Zhang, Appl. Phys. Lett. 73, 3049 (1998).
2
broadband THz radiation, the PC antenna works as an R. Huber, A. Brodschelm, F. Tauser, and A. Leitenstorfer, Appl. Phys.
integrating detector. The photocurrent from the antenna, J共t兲, Lett. 76, 3191 (2000)
3
is proportional to the time integration of the product of the M. C. Beard, G. M. Turner, and C. A. Schmuttenmaer, J. Phys. Chem. B
106, 7146 (2002).
incident THz electric field, E共t兲, and the total number of 4
M. Tani, S. Matsuura, K. Sakai, and S. I. Nakashima, Appl. Opt. 36, 7853
photo-generated carriers, N共t兲, in the PC antenna: J共t兲 (1997).

= e␮兰−⬁ ETHz共t⬘兲N共t⬘ − t兲dt⬘ where e is the electron charge 5
G. Zhao, R. N. Schouten, N. van der Valk, W. Th. Wenckebach, and P.
and ␮ is the electron mobility in the LT-GaAs. Therefore, for C.M. Planken, Rev. Sci. Instrum. 73, 1715 (2002).
6
an ideal PC antenna with ultrashort carrier lifetime, J共␻兲 S. Kono, M. Tani, and K. Sakai, Appl. Phys. Lett. 79, 898 (2001); 77,
4040 ( 2000).
⬀ ETHz共␻兲; while for a PC antenna with a long carrier life- 7
T. A. Liu, M. Tani, M. Nakajima, M. Hangyo, and C. L. Pan, Appl. Phys.
time (for example, a semi-insulating GaAs PC antenna), Lett. 83, 1322 (2003).
J共␻兲 ⬀ ETHz共␻兲 / ␻. For ultrabroadband THz detection using a 8
Y. C. Shen, P. C. Upadhya, E. H. Linfield, H. E. Beere, and A. G. Davies,
PC antenna with a finite carrier lifetime, the sensitivity at Appl. Phys. Lett. 83, 3117 (2003).
9
higher frequencies is thus expected to decrease (we also note I. S. Gregory, C. Baker, W. R. Tribe, M. J. Evans, H. E. Beere, E. H.
that the structure of the PC receiver antenna may affect its Linfield, A. G. Davies, and M. Missous, Appl. Phys. Lett. 83, 4199
(2003).
spectral response, and that Kono et al.6 used a dipole-type 10
P. C. Upadhya, Y. C. Shen, A. G. Davies, and E. H. Linfield, Vib. Spec-
antenna, different from the bowtie-type PC antenna used trosc. 35, 139 (2004).
here). Nevertheless, PC detection still provides about eight 11
M. Dauchez, P. Lagant, P. Derreumaux, G. Vergoten, M. Sekkal, and B.
times better signal-to-noise-ratio (defined as the ratio of the Sombret, Spectrochim. Acta 50A, 105 (1994).

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