THZ Time Domain Spectroscopy Lab
THZ Time Domain Spectroscopy Lab
2 Measurement principle
Terahertz Time-domain spectroscopy is a pump-probe spectroscopy technique,
where broadband THz pulses are measured at different points in time, using e.g.
Free-space electro optic sampling (FSEOS). A typical time-domain signal and
its Fourier transform is presented in Figure 2. The probing makes it possible
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to fully describe the temporal profile of the wave, i.e. both its amplitude and
phase. A typical measurement is a two-step process. Firstly a measurement
of the setup is performed, i.e. without any sample, this is called the reference
measurement. The second measurement is done with a sample in the path of the
THz radiation, known as the sample measurement. By comparing the spectral
profile of the two measurements, one can extract the complex refractive index.
Figure 2: A typical TTDS time trace for sample and reference in transmission,
with their corresponding Fourier-Transform.
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tion measurements, with the exception of some special techniques (e.g. ATR),
requires a physical replacement of a mirror with a sample between the two mea-
surements. This replacement often adds to the complexity of the setup and it
introduces an uncertainty in the phase shift due the positional shift between
sample and mirror [2], creating a preference for transmission measurements.
Electromagnetic radiation is subject to attenuation, in an extreme case a
pulse is indistinguishable from the background noise. In the case of TTDS,
pulse attenuation due to absorptive materials can be lowered to an acceptable
level by reducing the thickness of the sample, however, thin samples are prone to
Fabry-Perot effects. For the most absorptive materials, reflection measurements
are necessary.
In TTDS both measured signals, reference and sample, are Fourier transformed
and compared through division,
Es (ω)
H(ω) = = T (ω)eiφ(ω) . (2)
Er (ω)
Here Es (ω) and Er (ω) are the Fourier transformed sample and reference pulse,
respectively. Where T (ω) is the amplitude and φ(ω) is the phase. Both the
amplitude and unwrapped phase of the Transfer function H(ω) for the signal in
Figure 2 is included in Figure 3. A similar discussion on extraction of optical
parameters from TTDS is described in [8].
Fresnel’s coefficients t12 and t21 are approximately real valued for low absorptive
samples. We can solve analytically for κ(ω) and n(ω),
φ(ω)c
n(ω) = + nair (4)
d
c (n(ω) + nair )2
κ(ω) = − ln [ T (ω)]. (5)
ωd 4n(ω)
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Figure 3: The top shows the amplitude of the transfer function, while the
bottom show the unwrapped phase. Unwrapping is used as a means of removing
unwanted discontinuities when the phase jumps one cycle, i.e. when the phase
reach ±2π.
These are the simplest expressions for n(ω) and α(ω) [6]. The resulting optical
parameters for the simulated signals in Figure 2 is shown in Figure 4.
The thickness is the biggest source of error in calculations of n and κ, which
will be addressed in the laboratory lesson.
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Figure 4: The Absorption coefficient and refractive index of the simulated sam-
ple in Figure 2. Calculated using equations (4) and (5). From the calculated
refractive index, we can see that the simulated sample is a Lorentz medium,
with the Lorentzian fixed around 2 THz.
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analytical. Numerical methods , such as Fixed-point iteration, become a neces-
sity to solve for the complex refractive index. We can represent the equations
by their measurable parts and their theoretical parts as follows,
4 p ω
T (ω) = 2 2
n(ω)2 + κ(ω)2 e− c κ(ω)d (6)
(n(ω) + 1) + κ(ω)
−κ(ω) ω κ(ω)
φ(ω) = arctan( ) + (n(ω) − 1)d + arctan( ).
1 + n(ω) c κ(ω)2 + n(ω) + n(ω)2
(7)
where T (ω) and φ(ω) can be the expressions shown in equations (6-7) or equation
(3), i.e. assuming absorptive or low-absorptive material. We can write the
Fabry-Perot terms as,
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X n(ω)ωd
F P (ω) = (r10 e−i c )2k . (9)
k=0
Here r10 is Fresnel’s reflection coefficient, and k is the k’th Fabry-Perot reflec-
tion term, whilst i is the maximum number of reflections, the case in Figure 5
gives i = 2. One possible approach to remove FP effects numerically is proposed
in [8], this method is based around making a guess for n and κ, which normally
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Figure 5: (TOP) Fabry perot time trace from 300µm GaP (The EO-detection
crystal) (BOTTOM) The absolute value of the Discrete Fourier Transform of
the pulse train.
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is done with equations (4-5). Afterwards for each frequency a numerical method
is applied to minimize the error between the measured transfer function and the
analytic, see [9, 8]. Any such numerical solution is not necessary for complet-
ing the laboratory lesson, but it is important that the student understand the
limitations imposed by limiting the time window.
Figure 6: Scheme for FSEOS, an optic sampling pulse and a pump THz pulse
propagates collineraly towards an electro-optic medium, the outgoing pulse from
the EO medium propagates through a compensator, typically a λ4 waveplate.
The wollaston prism (polarizing beam spltter) creates a decomposition of the
pulse in y and x directions. These pulses are fed to two photo-diodes which
are cross connected to an anode and cathode, resulting in balanced detection
I = Iy − Ix . Figure is from [1]
Iy − Ix = I ∝ ET Hz . (10)
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An important aspect to FSEOS is the alignment procedure, here one blocks
the THz-Pulse shown in Figure 6, and align the λ/4-waveplate such that the
outgoing probe pulse is circularly polarized, making equation (10) equal zero.
After this alignment, one can unblock the THz pulse, and the detected signal is
solely due to the birefringence induced in the EO-crystal by the THz pulse.
The tensor properties of the electrooptic crystal, implies that the orienta-
tion and crystal axes of the EO-crystal is vital to the nonlinear process in the
detection scheme. Two of the normal electro-optic crystal used in FSEOS are
ZnTe and GaP, both of zincblende structure (4̄3m). For the case of a h1 1 0i-
oriented zincblende crystal the THz field and the optical pulse should be aligned
in [1 1 0], and the optical pulse should be parallel to the THz field, to maximize
the birefringence in the zincblende electro-optic crystal [5].
5 Photoconductive antenna
The most widespread generation scheme of THz radiation is the photoconductive
antenna (PCA). The simplest version is shown in Figure 7. Two electrodes
are deposited onto a semiconductor substrate in which free carriers exhibit an
ultrashort lifetime. In the absence of any photo-excitation of charge carriers,
the semiconductor is highly resistive (intrinsic). Since no current flows between
the electrodes, it acts as a dipole, whose dipolar moment p is defined by the
charge difference and distance between the electrodes. In other words, the bias
voltage (DC-Bias) over the gap of distance W ,
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Now, a short optical pulse illuminates the region between the electrodes,
generating free carriers by photo-absorption. The photo induced carrier pop-
ulation first changes the permittivity of the semiconductor and subsequently
accelerates the carriers, whereof some reaches the electrodes. All these phenom-
ena creates a variation in the dipole moment over the electrode gap. It is this
variation which emitte the electromagnetic waves.
One can approximate the radiation from the PC antenna as a Hertzian dipole
where the antenna size is much smaller than the wavelength of the radiated
radiation. This is a valid approximation as the source size is approximately
the same size as the incoming optical pulse spot size (around 10µm), whilst
the wavelength of the THz wave is around 300µm for 1 THz [5]. By only
investigating the far field, i.e. where the propagation distance (r) is much bigger
than the wavelength of THz , we arrive at the equation for far field THz dipole
radiation in free space
2
~ T Hz = µ0 sin θ d [p(tr )]θ̂.
E (11)
4π r dt2r
Here θ is the angle between semiconductor front surface or i.e. the direction of
the THz radiation (θ = π2 for radiation as shown in Figure 7), p(tr ) is the dipole
moment of the source at the retarded time tr = t − r/c. Relating carrier density
ρ(r, t) to the dipole moment , and using the continuity relation
~ · J~ + dρ = 0.
∇ (12)
dt
We arrive at
dp(t)
= W IP C (t). (13)
dt
Where W is the spot size, which is approximated to be the same size as the
distance between the electrodes in Figure 7, and IP C is the photo-current. This
relates the emitted THz radiation to the time derivative of the current flowing
from one electrode to the other by
x
~ T Hz , we arrive at the relation
By investigating the Fourier-transform of E
ET Hz (ω) = ωµVDC−Bias Plaser . (15)
Here, we recognize that the THz electric field is proportional to the charge
mobility of the semiconductor µ, the applied electrode voltage VDC−Bias and
the incident laser power Plaser . This means, that the maximum radiation power
is limited by the breakdown voltage and the carrier mobility of the substrate
material. In addition to this, a high dark resistivity (short lifetime), is beneficial
such that there is no current before and after the laser pulse. Such that the
current pulse is as short as possible, and a broader spectrum of THz electric
can be generated. For more details, see [5].
6 Homework Problems
6.1 Free space electrooptic detection
We have already described the typical FSEOS setup (see Fig.6. Let’s assume
the incident detected intensity on each of the photodetectors (in balance) is I20 .
When the THz is incident on the ZnTe crystal, (polarization paralell to [110]),
each of the polarization is retarded, as a result of Pockel’s effect, by sin(∆φ),
such that
I0
Iy = (1 + sin(∆φ)), (16)
2
I0
Ix = (1 − sin(∆φ)). (17)
2
Show that the difference Iy − Ix is proportional to the THz electric field
ET Hz . HINT: You can assume the retardation to be very small. HINT2: You
need to consider the electrooptic tensor.
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6.4 Extraction of the optical parameters
Starting from
Es (ω)
H(ω) = = T (ω)eiφ(ω) . (19)
Er (ω)
Calculate extraction expressions for n and κ, for optically thick samples, low
absorptive samples. Explain what the different symbols in the equation mean,
and how they are related to the things we measure. What would happen if we
measured the absolute value |ET Hz | instead of ET Hz ?. HINT: You want to
arrive at the formulas in Section 3.1.
7 Laboratory Task
7.1 SAFETY
You will be working with a CLASS 4 Laser, meaning that it is in the class of
most dangerous Lasers. From Wikipedia: Lasers in this class have output
powers of more than 500 mW in the beam and may cause severe,
permanent damage to eye or skin without being focussed by optics
of eye or instrumentation. Diffuse reflections of the laser beam can
be hazardous to skin or eye within the nominal hazard zone. Many
industrial, scientific, military and medical lasers are in this category..
Generally, there will be a supervisor present during the lab, but there are
some general rules to be followed: (1) USE PROTECTIVE EYEWEAR
(2) DONT WEAR RINGS, WATCHES OR OTHER STUFF THAT
MAY REFLECT THE LASER LIGHT (3) DO NOT LOOK INTO
THE LASER BEAM, BEND DOWN TO LOOK AT STUFF IN THE
LASER BEAM HEIGHT OR PICK UP STUFF YOU LOST ON
THE FLOOR. Be careful.
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Figure 8: The Class 4 Laser, Tsunami, from spectra physics. Delivering over
500mW avarage power at around 80 MHz repition rate. The pulses are around
60 femtosecond in duration!
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Figure 9: PROTECTIVE EYEWEAR, should always be used.
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Figure 10: Experimental setup, THz-TDS. The first paraboloidal mirror is sit-
uated in such a way that they collect the radiation from the PCA such that it
is collimated. There is a focus in the region where the sample is situated. The
sample can move in and out of the THz path with a electrical motor. The THz
is then collimated again, before being focused and impinging on the Electrooptic
crystal. The probe beam, is propagating on the right hand side of the picture,
through the delay line and then through one of the last paraboloidal mirrors,
before meeting up with the THz radiation at the electrooptic crystal.
Two optical paths has to be considered in the optical setup, firstly, the THz
beam radiates from the PCA , and is collimated, focused, collimated and finally
focused again, by 4 off-axis paraboloidal mirrors. The first region of focus is
where the sample will be placed. The sample is mounted on a electric motor.
Secondly, the probe pulse, that is used to sample the THz by FSEOS is delayed
by a electrical motor, such that the THz electric field is detected as a function
of distance. This distance can easily be converted to time by considering the
velocity of light in air. All the pertinent programs are available on the computer
located next to the LIA/function generator. The programs are programmed
directly in MATLAB.
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7.3 Setting up the PCA
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Figure 12: Multimeter
Connect the multi-meter to the PCA BNC and measure the resistance with
no incident laser light on the Photoconductive Antenna.(Q1) Is the value rea-
sonable? (Q2) Why is it important with a large dark resistance? The equipment
is very expensive, be careful when connecting the BNC to the multimeter.
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Figure 13: BNC from PCA
We’re now interested in how the conductivity (i.e. resistance) changes when
a laser pulse is impinges on the surface of the antenna. You will now be handling
the laser beam itself, and it is important that you talk to your lab supervisor,
which will explain to you what to do. Measure the incident laser power before
the lens, this should be above 0.5W . Now, measure the resistance of the antenna.
(Q3) Why do you think the resistance change?
You will now put a bias over the electrodes of the antenna. The bias will be
modulated as a square wave by a signal generator, this modulation frequency
is fed into a Lock-in Amplifier to increase Signal-to-Noise ratio of the measure-
ments. The signal generator is situated on top of the Lock-in Amplifier as shown
in Figure.14
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Figure 14: Signal generator on top of the Lock-in amplifier
The Lock-in amplifier should be turned on, if not ask the lab supervisor to
help you. The power button of the signal generator is located on the front,
white button on the left of the grey panel. The modulation voltage should not
exceed 15V, as this is the limit of the PCA. (Q4) What sets the limit of the Bias
Voltage? (Q5) How would you expect the THz power to change with increasing
DC-voltage? Set the voltage to a reasonable amount, so that you may increase
it later, but not beyond 15 Volt. You need to turn on the output, but for now
you can keep it off.
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Figure 15: The photodetectors used for balanced detection
See if you can see the beams that are hitting the two detectors. (Q7)
Explain the difference in polarization between them. (Q8) When comparing to
the homework, what does these beams represent?
We will now lock-in to another reference, namely a chopper reference. Con-
nect the chopper output trigger to the lock-in input trigger. Turn on the chopper
and verify that the trigger works. (Q9) Do you see any signal on the lock-in?
(Q10) What happens if you block one of the photo-detectors? Reason. (Q11)
What would happen if you rotate wave-plate in the polarization sensitive detec-
tion setup?
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7.6 Rotating the ZnTe and ramping DC-bias
As you are resting the delay line on the peak, rotate the ZnTe crystal. (Q12)
Make a graph and explain what you observe. (Q13) Make a graph of THz
power as a function of DC-bias DO NOT EXCEED 15V.
7.8 Analysis
There are multiple ways of getting rid of the spectral ringing. One way is to limit
the scan region. There are two trivial ways of doing that. (a) Physically, but
shortening the delay line scan or (b) post-processing by limiting the time vector
in the program. Either way is fine. (Q17) Use one of these approaches and
explain how it affects the resolution and bandwidth of the experiment. (Q17)
What kind of limits does this set on the experiment? You can use the program
Extraction.mat to extract n and κ. (Q18) Compare your values to literature
and explain possible discrepancies.
References
[1] http://photonicswiki.org/images/e/eb/FSEOS of THz.png. Checked
09.09.2019.
[2] H. Němec F. Kadlec A. Pashkin, M. Kempa and P. Kužel. Phase-sensitive
time-domain terahertz reflection spectroscopy. REVIEW OF SCIENTIFIC
INSTRUMENTS, 74(11), 2003.
[3] L. Duvillaret, F. Garet, and J. L. Coutaz. A reliable method for extrac-
tion of material parameters in terahertz time-domain spectroscopy. IEEE
Journal of Selected Topics in Quantum Electronics, 2(3):739–746, Sep 1996.
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[4] Lionel Duvillaret, Frédéric Garet, and Jean-Louis Coutaz. Highly precise
determination of optical constants and sample thickness in terahertz time-
domain spectroscopy. Appl. Opt., 38(2):409–415, Jan 1999.
[5] Yun-Shik Lee. Principles of Terahertz Science and Technology. Springer,
2009.
[6] David G. Cooke Peter Uhd Jepsen and Martin Koch. Terahertz spec-
troscopy and imaging – modern techniques and applications. Laser Pho-
tonics Rev, 5:124–166, 2011.
[7] Rohit P. Prasankumar and Antoinette J . Taylor. Optical Techniques for
Solid-State Materials Characterization. CRC Press, 1st edition, 2011.
[8] Maik Scheller. Data extraction from terahertz time domain spectroscopy
measurements. Journal of Infrared, Millimeter, and Terahertz Waves,
35(8):638–648, 2014.
[9] Trygve Sørgård. ”terahertz time-domain spectroscopy of thin material sam-
ple, master’s thesis. Norwegian University of Science and Technology, 2015.
[10] Withawat Withayachumnankul and Mira Naftaly. Fundamentals of mea-
surement in terahertz time-domain spectroscopy. Journal of Infrared, Mil-
limeter, and Terahertz Waves, 35(8):610–637, Aug 2014.
8 Appendix
8.1 Unwrapping and Extrapolation of phase and the im-
pact on n and κ
This section is all about the phase φ(ω) term in the following equation
Es (ω)
H(ω) = = T (ω)eiφ(ω) . (20)
Er (ω)
φ is describing the ratio between the complex and real part of the trans-
fer function trough an angle in complex space. Using the phase term directly
in calculations of n and κ gives discontinuities phase jumps due to the phase
jumping from −π to π or vice versa. To prevent this, one use unwrapping which
makes the phase term continuous. Unwrapping is done by adding/subtracting
2π as the phase is 2π shifted each jump.
However, this may impose a 2πn bias in the phase throughout the whole
spectrum. Specially in the lower frequencies as there are more uncertainty in
the measurement due to lower spectral amplitude. A discussion on this can also
be found in [10].
Some authors argue that using a linear extrapolation from the middle fre-
quencies, where the phase is set to zero at ω = 0 is a good solution. This solution
is used by some authors and is discussed in detail in [3]. In this lab we do not
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use any extrapolation. However, for the readers appreciation we have included
two figures that show how this impacts n and κ for a particular measurement
in this setup.
We extrapolated the measurement by using the phase between 0, 09 to
4.5THz. Then we use the extrapolated values for frequencies below 0.09THz.
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Figure 16: (TOP) Extrapolated phase and initial phase (MID) n for both cases
(BOT) Absorption coefficient for both cases.
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