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An ultrafast terahertz scanning tunnelling microscope

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 LETTERS
PUBLISHED ONLINE: 7 JULY 2013 | DOI: 10.1038/NPHOTON.2013.151
An ultrafast terahertz scanning
tunnelling microscope
Tyler L. Cocker1 *, Vedran Jelic1, Manisha Gupta2, Sean J. Molesky2, Jacob A. J. Burgess1,
Glenda De Los Reyes1, Lyubov V. Titova1, Ying Y. Tsui2, Mark R. Freeman1 and Frank A. Hegmann1 *
Ultrafast studies1,2 of excitations on the nanometre scale are
essential for guiding applications in nanotechnology. Efforts
to integrate femtosecond lasers with scanning tunnelling
microscopes (STMs)3 have yielded a number of ultrafast STM
techniques4–14, but the basic ability to directly modulate the
STM junction bias while maintaining nanometre spatial resol-
ution has been limited to ∼10 ps (refs 7,8) and has required
specialized probe or sample structures. Here, without any
modification to the STM design, we modulate the STM junction
bias by coupling terahertz pulses to the scanning probe tip of an
STM and demonstrate terahertz-pulse-induced tunnelling in an
STM. The terahertz STM (THz-STM) provides simultaneous
subpicosecond (<500 fs) time resolution and nanometre (2 nm)
imaging resolution under ambient laboratory conditions, and
can directly image ultrafast carrier capture into a single InAs
nanodot. The THz-STM accesses an ultrafast tunnelling regime
that opens the door to subpicosecond scanning probe microscopy
of materials with atomic resolution.
Purely electronic techniques for modulating the tip bias for time-
resolved scanning tunnelling microscopy (STM) have been limited
to times greater than 0.3 ns (refs 15–17). Using femtosecond laser
pulses to photoconductively gate the signal in a specially modified
GaAs scanning probe tip, a time resolution of 2 ps and spatial
resolution of 20 nm have been achieved10. However, capacitive
coupling effects have been shown to limit the performance of photo-
conductively-gated STM9. Junction-mixing STM6–8, which uses
photoconductive switches and microstrip transmission lines
patterned on the sample to transport picosecond voltage pulses to
the tunnel junction, has shown spatial resolutions down to 1 nm
with time resolutions on the order of 10 ps, limited by the micro-
strip bandwidth7,8. Focusing time-delayed femtosecond laser pulse
pairs on the tip–sample junction modifies the tunnel current
through sample excitation, but can also result in optical-pulse-
induced thermal expansion effects4,13, although recent schemes
have managed to reduce such artefacts11–14. Autocorrelations of
optically induced STM signals with subpicosecond widths
have been shown11–14, and shaken pulse-pair-excited STM has
recently been used to image ultrafast dynamics in real space with
nanometre resolution11.
Coupling free-space terahertz pulses to an STM tip (THz-STM)
offers a new possibility for modulating the tip bias that avoids limit-
ations from capacitive coupling, microstrip bandwidth and thermal
expansion. Terahertz pulses have been used extensively for probing
ultrafast carrier dynamics in materials with diffraction-limited
spatial resolution (1 mm)1,2,18,19. Significant advances have also
been made in terahertz near-field imaging using scanning probe
tips19–23 with 40 nm spatial resolution22, but ultrafast time resolution
has not yet been demonstrated in a pump–probe geometry. The
1
Department of Physics, University of Alberta, Edmonton, Alberta T6G 2E1, Canada, 2 Department of Electrical and Computer Engineering, University of
Alberta, Edmonton, Alberta T6G 2V4, Canada. * e-mail: tcocker@gmail.com; hegmann@ualberta.ca
620
© 2013 Macmillan Publishers Limited. All rights reserved.
THz-STM combines the high spatial resolution of an STM with
the subpicosecond time resolution of terahertz pulse spectroscopy.
It uses the nonlinear current–voltage (I–V ) relation of the tip–
sample tunnel junction to produce a rectified ultrafast tunnel
current burst in a process reminiscent of junction-mixing STM6–8.
However, free-space coupling of terahertz pulses in the THz-STM
requires no modifications to the STM design or sample. As a
result, the THz-STM achieves a time resolution of ,0.5 ps, much
faster than that reported for junction-mixing STM or photoconduc-
tively gated STM, while maintaining nanometre spatial resolution.
Furthermore, because terahertz pulses coupled to the STM tip act
like fast voltage transients that sample the I–V curve of the tunnel
junction with subpicosecond time resolution, time-resolved
pump–probe experiments with the THz-STM provide a direct
picture of excitation dynamics and apply to a wide range of
sample excitations.
The basic operation of the THz-STM is described in Fig. 1. An
ultrafast laser source generates free-space-travelling terahertz pulses
(Fig. 1a) that are then focused onto the scanning probe tip of an
STM (Fig. 1b). The STM tip essentially acts like a broadband
antenna21,24 that couples the electric field of the terahertz pulse to
the tunnel junction (Fig. 1c) via a Sommerfeld mode25. The total
time-dependent voltage V(t) across the tunnel junction (Fig. 1d) is
then the sum of the d.c. bias voltage V0 and the transient voltage
VTHz(t) arising from the tip-coupled terahertz pulse. Thus, a free-
space terahertz pulse coupled to an STM tip behaves like an ultrafast
voltage transient and drives electrons across the junction. The
characteristic nonlinear I–V relation of the STM tunnel junction
results in a time-dependent tunnel current  response I(t) ¼ I0 þ
ITHz(t) with a rectified component (that is, ITHz(t)dt = 0), as illus-
trated in Fig. 1e, where I0 is the STM tunnel current setpoint.
Although the STM electronics are far too slow to resolve the sub-
picosecond features of the terahertz-induced current pulse, the
STM is capable of measuring the time-averaged shift in tunnel
current due to the rectified component. Furthermore, because the rec-
tified component of the current response is generated at the tunnel
junction itself, the spatial resolution of the THz-STM is defined by
the tunnel junction area. The scale of the terahertz-induced
changes to the average tunnel current can be seen in the STM I–V
curves taken over a bare, flat, highly ordered pyrolytic graphite
(HOPG) test sample, as shown in Fig. 1f. Terahertz pulses were
found to produce an increased current when the terahertz-pulse elec-
tric field is polarized parallel to the STM tip. On the other hand, the
terahertz-induced tunnel current disappears when the pulse is polar-
ized perpendicular to the tip, consistent with polarization-dependent
terahertz coupling to antennas or metal wires21,24,25. We confirmed
that the terahertz-induced tunnel current was not due to tip
thermal expansion effects (see Supplementary Information).
NATURE PHOTONICS | VOL 7 | AUGUST 2013 | www.nature.com/naturephotonics
NATURE PHOTONICS DOI: 10.1038/NPHOTON.2013.151 LETTERS
a b c

Amplitude
4 A
V0
Electric field (a.u.)

2
0 1 2 3 40° 0.25 mm
Frequency (THz)
0 2 mm

−2

Pl/Ir tip
−4
E
0 4 8 12
Time (ps) Sample

d e f
V0 + VTHz(t) I 4
0.4 P
I0 + ITHz(t)
Total voltage (V)

V0 2

Current (nA)
0.2
Vertical
0.0 0 polarization
V P
−0.2 −2

−0.4 Horizontal polarization

−4 Pulse blocked
V0 + VTHz(t)
0 4 8 12
Time (ps) −0.10 −0.05 0.00 0.05 0.10
Bias voltage (V)

Figure 1 | Coupling terahertz pulses to a scanning tunnelling microscope (THz-STM). a, Electric field of a terahertz pulse measured by free-space electro-
optic sampling. Inset: corresponding frequency spectrum of the terahertz pulse. b,c, Terahertz pulses propagating through free space are focused onto the
STM tip (b) and couple to the Pt/Ir STM tip wire at an angle of 408 above the horizontal with a spot size on the order of 2 mm (c). The electric field of
the coupled terahertz pulses is enhanced at the end of the STM tip. d, The total voltage applied across the tunnel junction is the sum of the STM bias
voltage (V0) and the time-dependent voltage due to the coupled terahertz electric field (VTHz(t)). e, The tunnel current is nonlinear as a function of total
voltage across the junction, so the bias voltage ensures that the terahertz-induced tunnel-current response is asymmetric. Therefore, the terahertz-induced
tunnel current contains a measurable, rectified component. f, STM I–V curve over HOPG with terahertz pulse polarization parallel (vertical polarization, blue
solid line) and transverse (horizontal polarization, red solid line) to the STM tip. The I–V curve with the terahertz beam blocked is shown by the green
dashed line. The peak electric field of the terahertz pulse was 0.120 kV cm21 for both horizontal and vertical coupling polarizations. The feedback loop
remained off during the I–V measurement. Measurements were performed in air, at room temperature.

A terahertz pulse autocorrelator was used to test the time resol-
ution of the THz-STM, as shown schematically in Fig. 2a. Gold
nanoislands were deposited on an HOPG substrate to provide
THz-STM signal contrast through I–V curve differences. THz-
STM autocorrelations measured with the tip located over one of
the gold nanoislands and over the bare HOPG substrate are
shown in Fig. 2b–d and Fig. 2e–g, respectively. Extremely large
tunnel currents are achieved during the ultrafast duration of the
THz pulse. To access such currents, the terahertz voltage applied
to the tunnel junction must be large relative to the d.c. bias
voltage. The approximate current–voltage relation of an STM
tunnel junction can be described over a wide voltage range by the
Simmons model26. At voltages larger than the sample and tip
work functions, the tunnel barrier effectively narrows and tunnel-
ling field emission occurs3, which leads to a large increase in
current. The THz-STM operates in this extreme tunnelling
regime, where milliamp tunnel currents can be reached on subpico-
second timescales. Simulations of the overlap of two terahertz pulses
at the junction, where the I–V curves are described by the Simmons
model, provide very good agreement with the observed measure-
ments. The model gives a terahertz electric field enhancement at
the tip of 8,000, resulting in effective terahertz voltages of 0.3–
0.4 V (see Supplementary Information). Figure 2h shows the
onsets of the THz-STM signals over the gold nanoisland and the
HOPG substrate, as determined from the peak values of Gaussian
fits to the observed autocorrelations, which closely follow the
Simmons model predictions. Figure 2i plots the full-width at half-
maximum (FWHM) values of the Gaussian fits to the observed
autocorrelations in Figs 2b–g, providing an estimate of the timescale
over which the rectified electrons are generated. Autocorrelation
widths as small as 350 fs FWHM over gold are observed.
The gold nanoisland sample was also used to test the simul-
taneous spatial and temporal resolutions of the THz-STM. Signal
contrast between the nanoislands and substrate was optimized by
fine-tuning the terahertz electric field strength close to
0.08 kV cm21 (Fig. 2h). THz-STM images of gold nanoislands on
the HOPG surface were taken as a function of autocorrelation
overlap time, as shown in Fig. 3a-d. The spatial resolution of the
THz-STM is determined from the edge definition of the gold
nanoislands in a linescan cut through the centre THz-STM image
in Fig. 3b, as shown in Fig. 3e, and is comparable to the resolution
of the STM topography images in Fig. 3a. As a near-field imaging
technique using broadband terahertz pulses at 1 THz (l ¼
300 mm), the THz-STM achieves l/150,000 spatial resolution.
Overall, Fig. 3 demonstrates the simultaneous ultrafast temporal res-
olution (≤500 fs) and nanometre spatial resolution (2 nm) of the
THz-STM under ambient laboratory conditions. Based on these
measurements, the resolution of the THz-STM appears to be
limited only by the spatial variation of the I–V curve and the
imaging resolution of the STM itself.
To demonstrate the ability of the THz-STM to probe ultrafast
carrier dynamics in a single nanoparticle with subpicosecond time
resolution, we performed an optical-pump/THz-STM-probe exper-
iment on a sample with InAs nanodots grown on GaAs.
Simultaneous STM and THz-STM images of the InAs nanodot
sample surface were taken at negative time delays with the terahertz

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LETTERS NATURE PHOTONICS DOI: 10.1038/NPHOTON.2013.151

a b Au e HOPG
THz peak field THz peak field

electrons/pulse

electrons/pulse
4,000 4,000
74 V cm−1 87 V cm−1

Rectified

Rectified
2,000 2,000

0 0
−1 0 1 −1 0 1
Autocorrelation Autocorrelation
overlap time (ps) overlap time (ps)

c f
78 V cm−1 92 V cm−1

electrons/pulse

electrons/pulse
4,000 4,000

Rectified

Rectified
2,000 2,000
h
Autocorrelation peak
(rectified electrons)

4,000 Au nanoisland
HOPG 0 0
2,000 −1 0 1 −1 0 1
Autocorrelation Autocorrelation
0 overlap time (ps) overlap time (ps)

0.00 0.04 0.08 d g

83 V cm−1 97 V cm−1

electrons/pulse

electrons/pulse
THz peak field (kV cm−1) 4,000 4,000

Rectified

Rectified
i 2,000 2,000
Autocorrelation

Au nanoisland
FWHM (ps)

0.5
HOPG
0.4 0 0
−1 0 1 −1 0 1
0.3
Autocorrelation Autocorrelation
overlap time (ps) overlap time (ps)
0.07 0.08 0.09 0.10
THz peak field (kV cm−1)

Figure 2 | Autocorrelation of terahertz pulses at an STM tunnel junction. a, Schematic of the terahertz pulse autocorrelator. A silicon wafer is used as the
beamsplitter. b–d, Amplitude of the THz-STM signal (rectified electrons per terahertz pulse) over a gold nanoisland as a function of autocorrelation overlap
time for terahertz pulses with peak electric fields (at full overlap) of 74 V cm21 (b), 78 V cm21 (c) and 83 V cm21 (d). e–g, THz-STM autocorrelation over
the HOPG substrate for terahertz pulses with peak electric fields of 87 V cm21 (e), 92 V cm21 (f) and 97 V cm21 (g). For all measurements the bias voltage
was þ30 mV and the tunnel current setpoint was 1.0 nA. All autocorrelations were measured in air, at room temperature. Solid lines that are the same colour
as the data are Simmons model fits based on terahertz-pulse-induced current rectification (see Supplementary Information). Grey lines are Gaussian fits
to the autocorrelation data. h, THz-STM signal onsets over the gold nanoisland and the HOPG substrate as a function of terahertz peak electric field.
Experimental data points (squares, triangles) were determined from the Gaussian fits to the observed autocorrelation peaks. Simmons model simulations of
the THz-STM signal onsets for the parameters determined from the autocorrelation fits are denoted by solid lines. i, FWHM values of the Gaussian fits to
the measured autocorrelations.

pulse arriving 500 fs before the 800 nm optical pump pulse (STM,
Fig. 4a; THz-STM, Fig. 4b; schematics, Fig. 4c,d) and at positive
time delays with the terahertz pulse arriving 500 fs after the
optical pump pulse (STM, Fig. 4e; THz-STM, Fig. 4f; schematics,
Fig. 4g,h). The changes to the terahertz-induced tunnel current
caused by photoexcitation of the InAs nanodot result in a clear con-
trast between the THz-STM images resolved at positive and negative
time delays. In particular, ultrafast electron trapping in the InAs
nanodot10,27–29 increases the THz-STM signal, while the signal
above the surrounding InAs wetting layer remains relatively
unchanged. The edge resolution of the InAs nanodot is 6 nm in
Fig. 4f, as shown in Fig. 4i (also see Supplementary Information),
and the time resolution of the image is ≤1 ps (as demonstrated by
comparison of Fig. 4b with Fig. 4f ). The STM tip was then moved
to a location above the InAs nanodot, and the optical-
pump/THz-STM-probe signal was measured as a function of
pump–probe time delay, as shown in Fig. 4j. An optical-
pump/THz-STM-probe scan obtained by averaging five scans
over a different InAs nanodot is shown in Fig. 4k (two scans were
averaged for Fig. 4j). The rise time of the photoinduced THz-
STM signal is 500 fs. The decay time of the transient THz-STM
response of the InAs nanodot is 1 ps, which agrees well with
hole capture times reported in the literature10,27–29. The hole
capture time is slower than the electron capture time due to the
presence of a potential barrier in the hole energy landscape,
which arises from strain extending laterally around the
nanodot10,30. Therefore, for 1–2 ps after photoexcitation, the
InAs nanodots are negatively charged10. With negative d.c. sample
bias, charging increases the total voltage between the sample and
tip at the InAs nanodot and enhances the THz-STM signal
locally. The signal enhancement mechanism is depicted schemati-
cally in Fig. 4g,h. Finally, the nanodot size, shape and surface
density measured via scanning electron microscopy (SEM, Fig. 4l)
are consistent with the STM images.
The THz-STM can be easily applied to existing STM systems
without modification, and, in principle, be used to image the ultrafast
pump–probe I–V curve dynamics in a wide range of STM-
compatible samples while simultaneously recording STM topography
images at normal scan rates. All the experiments described in this
Letter were performed in air, but it is expected that moving the
set-up into vacuum will yield better signal stability and permit use
of the full dynamic range of the signal for contrast in THz-STM
imaging. The ultrafast charging dynamics of a single InAs nanodot
were shown with nanometre spatial resolution, but there is no appar-
ent intrinsic limitation that would prevent the THz-STM from
ultimately measuring subpicosecond charging dynamics of single
atoms or molecules. Coupling ultra-broadband terahertz pulses1,2
to the STM tip may improve the time resolution to ,100 fs.
We believe that the THz-STM will be an essential tool for spatially
resolving ultrafast dynamics within nanoscale device structures.

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NATURE PHOTONICS DOI: 10.1038/NPHOTON.2013.151 LETTERS
a
100 nm

13 nm

0 nm

b
4,500 e

−1,500 e

electrons
Rectified
2,000

0
−500 −250 0 250 500
Autocorrelation overlap (fs)

0.1
d

Electric field
(kV cm−1)
0.0

−0.1
0 2 4 6 0 2 4 6 0 2 4 6 0 2 4 6 0 2 4 6
Time (ps)

e
10,000
electrons
Rectified

2.8 nm
1.6 nm
5,000
HOPG
Gold
Gold
0
100 nm 0 5 10 15 20 25 30
Distance (nm)

Figure 3 | THz-STM imaging as a function of terahertz pulse autocorrelation overlap time. a, STM topography images of two gold nanoislands on an
HOPG surface. b, Corresponding THz-STM images, detected simultaneously. Images were measured with autocorrelation overlap time delay settings of
(from left to right) 2500 fs, 2250 fs, 0 fs, þ250 fs and þ500 fs. The colour scale represents the number of rectified electrons in the THz-STM signal,
where e is the fundamental charge. c, THz-STM autocorrelations measured over the upper left gold nanoisland (blue line, location indicated by blue circle in a)
and the HOPG substrate (green line, location indicated by green circle in a). The autocorrelation time axis indicates the autocorrelation overlap setting for
each of the images above. d, Corresponding terahertz autocorrelator waveforms. The incident terahertz pulse peak field was 0.08 kV cm21 at 0 fs
autocorrelation overlap. e, A linescan cut through the 0 fs-delay THz-STM image shows a nanoisland edge definition of 2 nm (blue shaded regions).
All measurements were taken in air, at room temperature, and at a bias voltage of þ30 mV and current setpoint of 1.0 nA.

Materials and methods
Sample fabrication. The gold nanoisland sample was made by evaporating 3 nm of
gold onto an HOPG substrate (the thickness refers to a uniform layer) under a
pressure of 1026 torr. The InAs nanodots were grown by solid source molecular
beam epitaxy on an epi-ready n-type (100) GaAs wafer (doping, 5 × 1017 cm23)
using the Stranski–Krastanov (SK) growth mode. The oxide from the GaAs substrate
was desorbed by heating it to 615 8C for 10 min with an arsenic pressure of 5 ×
1026 torr. No GaAs buffer layer was grown. Surface roughness can be attributed to
desorption of oxide from the GaAs surface. Growth of the InAs nanodots was
conducted at a substrate temperature of 520 8C with an In-to-As flux ratio of nearly
30, and the sample was then cooled to room temperature in an arsenic pressure. The
arsenic pressure was nearly the same as the growth pressure until the substrate
temperature was 285 8C, and then the arsenic source was cooled. The typical size
of an InAs nanodot was 100 nm × 50 nm, and nanodot heights ranging from 5 nm
to 25 nm were found using STM imaging. A surface roughness on the order of a few
nanometres can also be seen in the STM images. Auger electron spectroscopy
confirmed that the nanodots were composed of equal parts In and As, and also
showed that the surrounding substrate was covered by an InAs wetting layer.
Ultrafast laser source and terahertz generation. The laser used for the THz-STM
experiments was a commercial Ti:sapphire regenerative amplifier (RegA/Coherent)
seeded by a mode-locked oscillator (Micra/Coherent). The amplifier produced 6 mJ
pulses with a centre frequency of 800 nm at a repetition rate of 250 kHz. The pulse
duration was set to 150 fs to optimize the performance of the terahertz source. A
large-area photoconductive antenna based on a 0.5-mm-thick semi-insulating (SI)
GaAs wafer was used for terahertz pulse generation. High-voltage pulses tunable up
to 260 V were applied via chrome–gold contacts across a 1 mm gap to produce
ultrafast current transients in the wafer that emitted terahertz pulses. The amplitude
and phase of the terahertz-pulse electric field were measured by electro-optic
detection in a 1-mm-thick [110] ZnTe crystal. Further electric field and energy
calculation details are provided in the Supplementary Information. The terahertz
beam was chopped at 1 kHz. The InAs nanodot sample was excited using 800 nm,
150 fs pulses with a fluence of 110 mJ cm22 (4 × 106 photons mm22).
A description of the optical set-up is given in the Supplementary Information.
Scanning tunnelling microscope. The STM used is a commercial system (RHK
UHV SPM 3000) with ultrahigh-vacuum capabilities, although the STM scan head

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LETTERS NATURE PHOTONICS DOI: 10.1038/NPHOTON.2013.151

a b c TH d
z VTHz(t)
13 nm 1,250 e I
800
nm
V
ITHz(t)
0 nm −125 e
t0 − 500 fs

e f g TH h
z
13 nm 1,250 e VTHz(t) I

800
nm V

0 nm −125 e ITHz(t)
50 nm
t0 + 500 fs − − − + − +
+

j 500 fs
i 2,000

Rectified electrons
6 nm InAs nanodot
1,000 InAs wetting layer
1,500

Rectified electrons
0
1,000
Wetting 10
Height (nm)

layer
InAs 5 500
nanodot
0
0
0 50 100 150 200
−2 0 2 4 6
Distance (nm)
Pump/probe time delay (ps)

450 fs

l k 2,500

1,000
2,000
Rectified electrons

1,500 100
0 5
1,000 Pump/probe time
delay (ps)

500

400 nm
0
−2 0 2 4 6
Pump/probe time delay (ps)

Figure 4 | Ultrafast photoexcitation of an InAs nanodot (optical-pump/THz-STM-probe). a–c, STM topography scan (a) and simultaneous THz-STM image
scan (b) of an InAs nanodot taken at negative time delay with the terahertz probe pulse arriving at the tip 500 fs before the nanodot is excited at time t0 by
an 800 nm, 150 fs optical pump pulse, as shown schematically in c. d, The terahertz-induced tunnel current at negative time delay contains only a small
rectified component. e–g, STM topography scan (e) and simultaneous THz-STM image scan (f) of the same area with the terahertz probe pulse arriving
500 fs after the arrival of the optical pump pulse (positive time delay), as shown schematically in g. h, Electron trapping into the InAs nanodots raises the
magnitude of the local bias voltage and results in an enhanced terahertz-induced tunnel current with a large rectified component. i, The edge definition of the
nanodot in the positive time delay THz-STM image in f is estimated to be 6 nm from a linescan cut through the image. The incident optical pump fluence
and terahertz probe peak field for the imaged nanodot were 110 mJ cm22 and 0.1 kV cm21, respectively. The bias voltage for the scans was 23.5 V and the
current setpoint was 0.5 nA. All STM/THz-STM data were measured in air. j, Optical-pump/THz-STM-probe measurement of the excitation and decay of the
InAs nanodot (black line) and wetting layer (green line) with t0 ¼ 0 ps. k, Averaged optical-pump/THz-STM-probe measurement taken over a different InAs
nanodot (bias voltage ¼ 23 V, current setpoint ¼ 0.5 nA, THz probe peak field ¼ 0.07 kV cm21, pump fluence ¼ 250 mJ cm22). The blue line is an
exponential fit with a decay time of 1 ps and a constant offset. The rise time of the photoinduced THz-STM signal is 500 fs. l, SEM image of the InAs
nanodot surface.
was removed from vacuum for the THz-STM experiments described here. The STM IVP 200 with a gain of 100 mV nA21, 1.5 pA noise at 1.5 kHz, and a bandwidth of
tips were 0.25-mm-thick Pt/Ir (90/10%), and were made using the cut–pull method 50 kHz. The terahertz pulse coupling angle of 408 was set by the clear aperture
by crimping and pulling Pt/Ir wire with pliers. The STM preamp was model RHK allowance of the RHK STM scan head (Fig. 1b,c). The optical pump pulses were

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NATURE PHOTONICS DOI: 10.1038/NPHOTON.2013.151
coupled collinearly into the terahertz beamline to avoid tip shadowing effects. Each
of the STM image scans shown was recorded in 15 min and the corresponding
THz-STM image scans were recorded simultaneously using a lock-in amplifier with
a time constant setting of 3 ms. Individual autocorrelations and pump–probe time-
delay scans took 2 min each, with a lock-in time constant of 300 ms. Two pump–
probe scans were averaged to produce Fig. 4j, while five scans were averaged for all
other autocorrelation and pump–probe scans shown. The number of electrons N
rectified by each terahertz pulse was determined from the average terahertz-induced
tunnel current DIavg by N ¼ (DIavg)/( frepe), where frep ¼ 250 kHz is the repetition
rate of the laser source and e is the electronic charge. Generally, DIavg/I0 ≈ 0.1 during
THz-STM operation, such that DIavg ≈ 0.1 nA when the current setpoint is 1 nA. For
every 0.1 nA increase in average current, 2,500 electrons are rectified by each
terahertz pulse.
Received 9 December 2012; accepted 16 May 2013;
published online 7 July 2013
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Acknowledgements
The authors thank S. Xu (Alberta Centre for Surface Engineering and Science, University
of Alberta) for scanning electron microscope imaging, Auger electron spectroscopy
measurements and analysis of the InAs nanodot sample. The authors also acknowledge
technical support from G. Popowich, D. Fortin and D. Mullin. This work was supported by
the Natural Sciences and Engineering Research Council of Canada (NSERC), the Canada
Foundation for Innovation (CFI), the Alberta Science and Research Investments Program
(ASRIP), the Informatics Circle of Research Excellence (iCORE) and the NSERC Nano
Innovation Platform (NanoIP).
Author contributions
T.L.C. designed and built the THz-STM set-up, and T.L.C. and F.A.H. wrote the manuscript
with contributions from all authors. T.L.C. and V.J. developed the THz-STM and carried
out experiments with support from J.A.J.B., G.D.L.R., L.V.T. and F.A.H. S.J.M. contributed
to the initial design phase of the THz-STM. M.G. and Y.Y.T. provided the InAs nanodot
sample and assisted in sample characterization. T.L.C. analysed the data, and V.J., T.L.C.
and M.R.F. developed the Simmons model simulation and fits to the data. F.A.H. initiated
and developed the THz-STM concept with contributions from M.R.F., helped design the
THz-STM set-up, and supervised the project. All authors contributed to discussions.
Additional information
Supplementary information is available in the online version of the paper. Reprints and
permissions information is available online at www.nature.com/reprints. Correspondence and
requests for materials should be addressed to T.L.C. and F.A.H.
Competing financial interests
The authors declare no competing financial interests.
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