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Application Note - High-Speed Asynchronous Optical Sampling
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Ultrafast time-domain spectroscopy
Ultrafast optical time-domain spectroscopy
with femtosecond lasers has been an important tool for researchers and industrial
screening engineers for more than two decades. Applications range from investigations of fundamental excitations and relaxation processes in gases, bulk solids and
nanostructures via picosecond ultrasound-based characterization of layer thicknesses,
e.g. in chip fabrication processes, to security screening and life-science applications
of terahertz radiation. The time-scales of
interest lie between a few tens of picoseconds and a few femtoseconds.
Thus, classical electronics are too
slow, and optical correlation techniques are
therefore the standard method of choice.
Conventional ultrafast time-domain spectroscopy is based on pump-probe schemes
in which a single femtosecond (fs)-laser
provides the pump and the probe pulses.
A pump pulse excites a sample under investigation and creates a non-equilibrium
state. The evolution of that state is interrogated using a time-delayed pulse that
probes the sample response as function
of time-delay versus the pump pulse.
Fig. 1: Acoustic response of gold nanostructures to impulsive optical
excitation showing signatures of a surface melting phase transition.
Within 2 hours, 76 traces of 1ns duration were acquired at
different temperatures using high-speed ASOPS. A comparable
experiment with conventional techniques would take a few days
to complete [3].
The time-delay is usually adjusted by varying the distances that the pulses travel and
thus their relative time-of-flight before arriving at the sample. Many data points are acquired at different time-delays to complete
a full measurement. In most cases one pulse
travels over a retroreflecting mirror whose
position can be modified using a motorized
translation stage or a vibrating membrane.
One drawback of such techniques is that
each time when the retroreflector is
moved for time-delay adjustment, the
measurement is halted and thus valuable
measurement time is lost. Another enormous disadvantage of mechanical delay-scanning devices is that their scanning speed
is limited by the weight of the optomechanical components. In most cases motorized
stages require approximately 10 seconds to
1 minute to acquire one transient. This is
unpractical for online signal monitoring and
optimization. Also, slow drifts in laser
power, technical noise and environmental
variations are not averaged out efficiently.
Especially if several tens of picoseconds are
scanned and multiple transients are averaged for noise reduction, measurement
times can approach several tens of minutes.
High-speed asynchronous optical sampling (ASOPS)
High-speed asynchronous optical sampling
circumvents these problems by eliminating
mechancial delay scanning devices from
ultrafast time-domain spectroscopy systems.
To this end two femtosecond lasers with repetition rates fR=1 GHz are employed that
are stabilized at an offset of ΔfR=10 kHz (offsets between 2 kHz and 20 kHz are possible).
The faster laser serves as the pump laser,
the slower one as the probe laser. As result
of the detuning, successive pairs of pump
and probe pulses arrive at the sample with
a delay that incrementally increases by 10 fs
with each pulse pair. Thus, the delay between pump and probe pulses is linearly
ramped from 0 to 1 ns. The ramp is reset
to zero whenever the faster pump laser
'overtakes' the probe laser after exactly
100µs (the inverse of ΔfR) and a new measurement cycle starts. The time-delay τ as
function of real-time t is given by a straight-forward linear relation: τ=(ΔfR/fR)×t.
See Fig. 2 for an illustration of the high-speed ASOPS time-delaying principle.
Fig. 2.: ASOPS scheme – the time delay between pump and probe pulses is scanned by slightly differing pulse repetition rates. The difference frequency ΔfR determines the scan rate, while the temporal measurement window is given by the inverse of the pulse repetition rate 1/fR.
In a high-speed ASOPS system, the pump
and probe pulses are applied to the sample
in exactly the same way as in standard
setups, except that they originate from two seperate femtosecond lasers. The probe
laser is detected using a fast photoreceiver
and digitized with a fast A/D converter as a
function of real-time. The real-time scale is
then simply converted to a time-delay scale
by applying a scaling factor ΔfR/fR.
High-speed ASOPS permits a boost to
ultrafast measurement techniques that is
probably comparable to the step from an
analog data plotter to a digital sampling oscilloscope. High-speed ASOPS permits to
scan a 1 ns time-delay window at a rate between 2 kHz and 20 kHz, a performance that would be impossible with conventional techniques. The
time-delay resolution can be as low as 45 fs (see
discussion below). The high scan rate makes
online signal monitoring and optimimization
possible and permits to suppress technical
and environmental noise very efficiently. It
can also greatly enhance the data acquisition
speed of imaging applications of ultrafast
time-domain spectroscopy. Apart from a
much accelerated data acquisition, inherent
advantages of high-speed ASOPS are the
absence of changes in optical spot size at
the sample location and the absence of
pointing instabilities originating from the
scan unit. With indpendently tunable pump-and probe-lasers the realization of two-color experiments is straightforward,
providing additional versatility.
What determines the time-resolution?
In mathematical terms, the pulse pair-to-pair increment is given by ΔfR/fR2, representing the basic limit to the time-delay resolution of a high-speed ASOPS experiment. It amounts to 10 fs for fR=1 GHz and
ΔfR=10 kHz. Another limitation is given by
the available bandwidth B for signal detection and digitization. Suitable A/D converters with at least 14-Bit resolution are available with approximately 100 MHz sampling
rate. As result, in a system with ΔfR=10 kHz,
there are 10000 data points per 1 ns time-
delay window, or 1 datapoint each 100 fs. Similarly, in a system with ΔfR=2 kHz, there is 1 datapoint per each 20 fs.
The time-delay resolution resulting from B
can be written as Δτ=ΔfR/(fR×B). From the
above relations it becomes clear that repetition rates in the range of 1 GHz are favorable if a sub-picosecond time-delay resolution is required and a multi-kHz scanning
rate is to be maintained. The quality of the
feedback loop that controls the
offset frequency also crucially determines that time-delay resolution of high-speed ASOPS.
Gigaoptics' repetition rate offset locking unit
TL-1000-ASOPS is capable of maintaining a
45 fs time-delay resolution over the entire
available 1 ns measurement window.
Main building blocks for high-speed ASOPS
Main building blocks of a high-speed
ASOPS system are theGigajet TWINdual
femtosecond oscillator and theTL-1000-ASOPSrepetition rate offset locking unit. This
combination permits ultrafast pump-probe
experiments with the following features:
• no mechanical delay scanner
• real-time ultrafast spectroscopy
• 2-20 kHz scan rate
• 1-2 ns time delay window
• 45 fs typical time-delay resolution
• 1 GHz spectral resolution
• 6x10-7 t-1/2 signal resolution (5 mW probe
beam. t is averaging time in seconds [2].
• two-color pump-probe measurements
Fig. 3: Schematic of high-speed ASOPS based pump-probe system. This set-
up has been used to acquire the data shown in Fig. 1. Optical beam paths are red, electrical paths are black.
Fig. 4: Schematic ofHASSP-THz THz spectroscopy system. Optical beam paths
are red, electrical paths are black. Pump laser for Gigajet TWIN is not shown.
Applications
High-speed ASOPS can be applied whereever conventional ultrafast techniques are
used. The most wide-spread application is
ultrafast pump-probe spectroscopy. See
Fig. 3 for a typical setup of a high-speed
ASOPS pump-probe setup. Application
examples are spectroscopy of ultrafast
electronic and lattice dynamics in semiconductors [1,2], observation of structural dynamics in nanostructures [3], and investigations of multilayer-structures using picosecond ultrasound [4]. See Figs. 1,5 and 6
for signals
acquired with high-speed ASOPS. High-speed ASOPS is also highly suited for THz
time-domain spectroscopy, where the real-time capability is a great benefit for THz
based material investigation and screening
applications [2,5,6]. Specifically for THz
time-domain spectroscopy, Gigaoptics has
developed the transmission spectroscopy
systemHASSP-THz.It provides a convenient all-in-one solution for customers who
wish to purchase a ready-to-use high-speed
ASOPS spectrometer rather than spending
time to build their own device.
Fig. 5: Acoustic response of Si-on-insulator multilayer structure to optical excitation measured using a high-speed ASOPS pump-probe setup. The acquisition
time was 1 second. The dominating feature are recurring echos from the
Si-CoSi2 interface permitting to determine the Si layer thickness with sub-nm
precision [2,4].
Fig. 6: Reflectivity changes of a GaAs/AlAs superlattice after excitation with a 30fs pulse at 800nm.
Top window shows full signal. Center window shows extracted modulations of signal due to coherent phonon oscillations
with periods between 1ps and 20ps. Bottom window shows extracted modulations due to coherent LO phonons
at 8.8THz. This measurement demonstrates that
high-speed ASOPS can cover almost 5 orders of magnitude in time-delay.
Screen shot of HASSP-THz data acquisition and analysis software. Left panels
show full THz signal and zoom into first 100 ps. Right panels show FFT of time-
domain data and a sample transmission spectrum (sample was a cell with water
vapor at atmospheric pressure). Here, the acquisition time was set to 1 second,
i.e. each of the windows is updated at 1 Hz rate. Satellites on time-domain data
and modulations on spectrum are due to multiple reflection within THz emitter.
References
| [1] | A. Bartels et al., Appl. Phys. Lett. 88, 041117 (2006). |
| [2] | A. Bartels et al., Rev. Sci. Instrum. 78, 035107 (2007). |
| [3] | A. Plech et al., Nano Letters 7, 1026 (2007). |
| [4] | T. Dekorsy et al., Proc. SPIE 6393, 63930H-11 (2006). |
| [5] | C. Kistner et al., Appl. Phys. Lett. 90, 233902 (2007). |
| [6] | C. Janke et al., Opt. Lett. 30, 1405 (2005). |
| [7] | G. Klatt et al., Opt. Expr. 17, 22847 (2009). |
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Photograph of GIGAJET TWIN with dimensions 31cm × 36cm × 9cm. |
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Photograph of TL-1000-ASOPS repetition rate offset locking unit |
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