fast and sensitive terahertz detection using an antenna

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Fast and sensitive terahertz detection using an antenna-integrated graphene pn-junction Sebasti´ an Castilla, Bernat Terr´ es, Marta Autore, Leonardo Viti, Jian Li, § Alexey Y. Nikitin, k,Ioannis Vangelidis, # Kenji Watanabe, @ Takashi Taniguchi, @ Elefterios Lidorikis, # Miriam S. Vitiello, Rainer Hillenbrand, ,Klaas-Jan Tielrooij, *,,4 and Frank H.L. Koppens *,,ICFO - Institut de Ci` encies Fot` oniques, The Barcelona Institute of Science and Technology, Castelldefels (Barcelona) 08860, Spain CIC nanoGUNE, E-20018 Donostia-San Sebastian, Spain NEST, CNR - Istituto Nanoscienze and Scuola Normale Superiore, 56127 Pisa, Italy §State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China kDonostia International Physics Center (DIPC), Donostia-San Sebastin, Spain IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Spain #Department of Materials Science and Engineering, University of Ioannina, GR-45110 Ioannina, Greece @Advanced Materials Laboratory, National Institute for Material Science, 305-0044, Tsukuba, Japan 4Current address: Catalan Institute of Nanoscience and Nanotechnology (ICN2), Barcelona Institute of Science and Technology, Campus UAB, Bellaterra, Barcelona, 08193, Spain ICREA - Instituci´ o Catalana de Re¸ cerca i Estudis Avancats, 08010 Barcelona, Spain E-mail: [email protected]; [email protected] 1 arXiv:1905.01881v1 [cond-mat.mes-hall] 6 May 2019

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Page 1: Fast and sensitive terahertz detection using an antenna

Fast and sensitive terahertz detection using anantenna-integrated graphene pn-junction

Sebastian Castilla,† Bernat Terres,† Marta Autore,‡ Leonardo Viti,¶ Jian Li,§

Alexey Y. Nikitin,‖,⊥ Ioannis Vangelidis,# Kenji Watanabe,@ TakashiTaniguchi,@ Elefterios Lidorikis,# Miriam S. Vitiello,¶ Rainer Hillenbrand,‡,⊥

Klaas-Jan Tielrooij,∗,†,4 and Frank H.L. Koppens∗,†,∇

†ICFO - Institut de Ciencies Fotoniques, The Barcelona Institute of Science andTechnology, Castelldefels (Barcelona) 08860, Spain

‡CIC nanoGUNE, E-20018 Donostia-San Sebastian, Spain¶NEST, CNR - Istituto Nanoscienze and Scuola Normale Superiore, 56127 Pisa, Italy§State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and

Chemical Engineering, Nanjing University, Nanjing 210023, China‖Donostia International Physics Center (DIPC), Donostia-San Sebastin, Spain⊥IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Spain

#Department of Materials Science and Engineering, University of Ioannina, GR-45110Ioannina, Greece

@Advanced Materials Laboratory, National Institute for Material Science, 305-0044,Tsukuba, Japan

4Current address: Catalan Institute of Nanoscience and Nanotechnology (ICN2),Barcelona Institute of Science and Technology, Campus UAB, Bellaterra, Barcelona,

08193, Spain∇ICREA - Institucio Catalana de Recerca i Estudis Avancats, 08010 Barcelona, Spain

E-mail: [email protected]; [email protected]

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Abstract

Although the detection of light at terahertz (THz) frequencies is important for a large rangeof applications, current detectors typically have several disadvantages in terms of sensitivity,speed, operating temperature, and spectral range. Here, we use graphene as photoactive ma-terial to overcome all of these limitations in one device. We introduce a novel detector for tera-hertz radiation that exploits the photo-thermoelectric effect, based on a design that employs adual-gated, dipolar antenna with a gap of ∼100 nm. This narrow-gap antenna simultaneouslycreates a pn-junction in a graphene channel located above the antenna, and strongly concen-trates the incoming radiation at this pn-junction, where the photoresponse is created. Wedemonstrate that this novel detector has excellent sensitivity, with a noise-equivalent powerof 80 pW/

√Hz at room temperature, a response time below 30 ns (setup-limited), a high dy-

namic range (linear power dependence over more than 3 orders of magnitude) and broadbandoperation (measured range 1.8 – 4.2 THz, antenna-limited), which fulfills a combination thatis currently missing in the state of the art. Importantly, based on the agreement we obtainbetween experiment, analytical model, and numerical simulations, we have reached a solidunderstanding of how the PTE effect gives rise to a THz-induced photoresponse, which is veryvaluable for further detector optimization.

Photodetectors operating at THz frequenciesplay an important role in many applicationsin the fields of medicine, security, quality test-ing, chemical spectroscopy and more.1–7 One ofthe main benefits of THz radiation is its non-invasive nature and its capability to penetratemost dielectric materials, which are typicallyopaque at non-THz frequencies. For example,in the case of medical imaging and securityapplications, THz radiation offers clear advan-tages since it is non-ionizing due to its lowphoton energy (in the meV range) in contrastwith conventional X-ray radiation with muchhigher photon energy (in the keV range), lead-ing to strongly reduced health risks. Further-more, THz detectors are expected to play anenabling role for data communication at THzbit rates.8–10 For many of these applications,the ideal THz detector would meet the followingfive requirements: it should be highly sensitive(i.e. have a low noise-equivalent power, NEP),operate at room temperature, give a fast pho-toresponse, have a high dynamic range (therange between the lowest and highest measur-able incident light power), and work over abroad range of THz frequencies, in particularabove 1 THz.

Commercially available room-temperatureTHz detectors, for example pyroelectric detec-tors and Golay cells, are reasonably sensitive

with an NEP on the order of ∼1 nW/√

Hz.However, their response time is very long: 100and 30 ms, respectively.11,12 Bolometric THzdetectors, on the other hand, can be highlysensitive with an NEP of ∼0.5 pW/

√Hz, while

simultaneously showing fast operation with aresponse time of ∼50 ps. However, these detec-tors require cryogenic temperatures (∼4 K) andsuffer from a narrow dynamic range (maximumdetectable power ∼0.1 µW).13 Schottky diodes,although combining high speed (response timein the picoseconds regime) and high sensitiv-ity (NEP of 10 - 100 pW/

√Hz), have a low

frequency cut-off (operation only below ∼1THz) and a small dynamic range.14,15 Thus,currently there are no commercially availableTHz detectors that simultaneously meet all fiverequirements.

Owing to its exceptional optoelectronic prop-erties and broadband absorption spectrum(from the visible down to the GHz-THz range)graphene is a highly interesting photoactivematerial for detecting light.16–21 During thepast couple of years, there were several experi-mental demonstrations of graphene-based pho-todetection in the GHz-THz range. These de-tectors were based on various operating mech-anisms. First of all, there were reports de-scribing plasma wave-assisted THz detection,typically in the overdamped regime.20,22–25 This

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scheme has resulted in high sensitivities, withan NEP below nW/

√Hz, but typically this

mechanism is reported for radiation below 1THz. Secondly, ballistic graphene rectifierswere demonstrated with excellent sensitivity,but only operating below 1 THz.26 Moreover,a graphene-antenna coupled bolometer for de-tecting GHz radiation was shown with promis-ing values of sensitivity at low temperatures.27

Alternatively, one can exploit the photo-thermoelectric (PTE) effect, where absorbedTHz light heats up the graphene electrons,28

subsequently creating an electron-heat drivenphotoresponse if an asymmetry is present inthe device.29 Such an asymmetry could be cre-ated, for example, by using two different con-tact metals or by using two adjacent grapheneregions of different doping, e.g. forming a junc-tion. Photodetection based on the PTE ef-fect in graphene was first shown for visiblelight, where interband absorption of light oc-curs.30,31 More recently, also photoresponsesin the THz frequency regime, where absorp-tion occurs through intraband processes, wereattributed to the PTE effect.32,33 Moreover,several of the previously mentioned studies ex-ploiting alternative mechanisms also attributeda potentially significant fraction of the observedTHz photoresponse to the photo-thermoelectriceffect.20–26 Clearly, some controversy exist onwhich photoresponse mechanism dominates forgraphene excited by THz light, which has ham-pered the development of more optimized de-tectors. Furthermore, the main challenge forexploiting the PTE effect for THz detection isthe large mismatch between the large area ofthe incoming radiation and the small photo-active area of graphene, where the PTE effectoccurs.

Here, we solve this issue by introducing anantenna-integrated THz photodetector, basedon high-mobility, gate-tunable, hexagonal BN(hBN)-encapsulated graphene, where the in-coming THz radiation is concentrated suchthat it overlaps with the small photoactive areaof the graphene. Using the gate-tunability ofthe detector, we find that the PTE effect is the

dominant photoresponse mechanism. We sup-port this with a quantitative comparison of thedevice response with numerical simulations andan analytical model of the PTE photoresponse.We furthermore show that, owing to its noveldevice design, our PTE THz photodetectormeets all five requirements of an ideal detector.In addition, it has the advantage of being basedon low-cost materials with scalable integrationcapabilities with the well established CMOSelectronics for low-cost imaging systems.34 Fi-nally, it is very low in power consumption, asit is a passive device.

In the following, we will first explain how ourantenna-integrated pn-junction THz detectorworks, followed by the experimental charac-terization of the detector. Subsequently, weprovide an analytical model of the PTE detec-tor and numerical simulations of the absorp-tion enhancement of graphene induced by theantenna, and compare these results with theexperiments. Finally, we will compare the THzphotodection performance to the state of theart.

Our THz photodetector is based on a noveldesign (see Fig. 1a-c), which works as follows.The detector contains a dipole antenna thatis located ∼15 nm below a graphene channel.The antenna consists of two branches that areseparated by a very narrow gap, with a size onthe order of 100 nm. This antenna gap servesfor focusing the incoming THz radiation into avery small spot in the graphene channel. Here,the concentrated field of the antenna leadsto (intraband) absorption and the subsequentcreation of hot carriers.28 Since the creationof a photoresponse from hot carriers requiresa gradient in the Seebeck coefficient, we usethe antenna branches simultaneously as splitgates. We apply appropriate voltages (VL andVR) to the left and right antenna branch, andthrough capacitive coupling this creates a pn-junction in the graphene channel, and therebya THz-induced photoresponse. Thus, the an-tenna simultaneously creates the photoactivearea in the graphene channel (located aroundthe pn-junction, see Fig. 1c) and funnels inci-

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Page 4: Fast and sensitive terahertz detection using an antenna

Figure 1: a) Schematic representation (right; not to scale) of the antenna-integrated pn-junction device and azoom of the central part of the THz PTE detector (left; to scale), consisting of an “H-shaped” graphene channel,contacted by source and drain electrodes. Underneath the graphene channel, there are two antenna branches thatconcentrate the incident THz light around the antenna gap region. The color map superimposed on the device showsthe simulated power profile (|E/E0|2, where E0 is the incident electric field) at a position 5 nm below the graphenechannel. The black scale bar corresponds to 1.6 µm. b) Side view of the device design, with the superimposed colormap again indicating the normalized power profile as in panel a. The region where the field is strongly enhancedby the antenna overlaps with the central part of the graphene channel. c) Same as panel a, now indicating howthe antenna branches serve as local gates by applying voltages VL and VR. Appropriate voltages will create a pn-junction in the central part of the graphene channel, directly above the antenna gap (which is where incident THzlight is concentrated by the antenna). The color map superimposed on the device is a simulation that shows thephotoresponse created by local photoexcitation, varying the position of photoexcitation (see also SI). The largestphotoresponse is created when photoexcitation occurs around the junction region. The photoresponse then decreasesexponentially when moving away on both sides from the junction, with the exponential decay length given by thecooling length `cool. The photoactive area (dashed rectangle) therefore has a length 2 · `cool, and a width w, which isthe width of the central part of the graphene channel. d) Photocurrent image (log-scale) obtained by scanning thedetector in the focal plane of a focused laser beam at 3.4 THz. We use our QCL with an average power of 84.1 µW,and a peak irradiance in the center of the focus of 1200 W/m2. The THz light is polarized parallel to the antennaaxis. The observation of the Airy pattern with multiple observable rings indicates excellent detector sensitivity.

dent radiation to this photoactive area, due tothe very strong field enhancement of incidentTHz radiation above the gap between the twoantenna branches (see Fig. 1a-b).

Compared to previous antenna-integrated,graphene-based THz detectors,20–27 the ad-vantage of our design is that the antennagap is much smaller (100 nm vs. several mi-crons), which means that the THz intensityis greatly enhanced (∼4 orders of magnitude,see Fig. 1a). Also, there is no direct electri-

cal connection between the antenna and thegraphene, which means that there is no needfor impedance matching to assure current flowbetween antenna and graphene. The fact thatwe simultaneously use our antenna for focus-ing light and as split gate, has the advantagethat there automatically is very good overlapbetween the region where the incoming THzradiation is focused and the photoactive regionof the graphene channel (see Fig. 1a-c). Fur-thermore, we use hBN-encapsulated graphene,which leads to graphene with high mobility and

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low residual doping. This means that the re-sistance of the graphene channel will be low,and we can tune the system relatively close tothe Dirac point (point of lowest carrier density),where the Seebeck coefficient is largest. Finally,we pattern the graphene channel into an “H-shape” with a relatively narrow (micron-sized)width. The narrow width of the central partof the channel leads to an enhanced photore-sponse, as the hot carriers will have a highertemperature. The wider sides of the graphenechannel reduce overall device resistance by min-imizing contact resistance.

We have fabricated two “H-shaped”, high-mobility, hBN-encapsulated graphene deviceswith a dipolar antenna/gating structure, (seeMethods and Supporting Information for de-tails and optical pictures of the devices). Wemainly show the results obtained from THzphotodetector Device A and will mention someresults from THz photodetector Device B. BothDevice A and Device B have a width of thecentral part of the graphene channel (at thejunction) of w = 2 µm, whereas the gap sizesof the dipolar antennas are 200 and 100 nm,respectively. The vertical distance between an-tenna and graphene is given by the thickness ofthe bottom hBN layer, typically ∼15 nm, andthus small enough to warrant sufficient overlapbetween the electric field profile around the an-tenna gap, and the graphene (see also Fig. 1b).The graphene mobility for both devices is onthe order of 20,000 cm2/Vs, which is a lowerbound as it is determined from two-terminalmeasurements (see Supporting Information,SI). We characterize the performance of theTHz photodetector devices using two differentsetups, both containing a THz laser and opti-cal components to focus the light at our THzdetector. One setup contains a pulsed quan-tum cascade laser (QCL) operating at 3.4 THz,and two Picarin (tsupurica) lenses to focus thelight; the other setup contains a continuouswave THz gas laser with tunable output fre-quency, and a parabolic mirror to focus thelight (see Methods for details). The THz lightis usually modulated by an optical chopper andthe generated photocurrent is measured using

a pre-amplifier and/or lock-in amplifier. Weuse typical incident THz powers in the range ofseveral microwatts to several milliwatts.

We first scan our photodetector (Device A)across the THz focus using motorized stages(in the QCL setup, see Methods). The dipolarantenna, with a length of 60 µm, is smallerthan the THz focus (FWHM ∼200 µm), al-lowing us to spatially map out the intensity ofthe THz focus through the photocurrent IPTE.The results show a clear Airy pattern (see Fig.1d), where we are able to observe several ringsof the diffracted beam pattern. This suggeststhat our THz photodetector is very sensitive,considering that these rings contain only a verysmall fraction of total incident power of theTHz beam (Pin = 84.1 µW).

Before proceeding with quantifying the sensi-tivity, we first exploit the gate-tunability toidentify the photocurrent generation mech-anism and determine the optimal operatingpoint of our THz detector, by mapping out thephotoresponse as a function of gate voltages VL

and VR (see Fig. 2a). These measurements weredone with the THz gas laser at 2.52 THz, andusing Device A. The gate voltages indepen-dently control the carrier density (Fermi en-ergy) of the two graphene regions and thereforethe Seebeck coefficients S1 and S2. The Seebeckcoefficient of graphene has a non-monotonousdependence on carrier density, where it firstincreases upon approaching the Dirac pointand then changes sign when crossing the Diracpoint, i.e. when going from hole to electrondoping or vice versa (see Fig. 2b). Since thegenerated photocurrent IPTE ∝ (S1 − S2), thisleads to the characteristic sixfold pattern, firstshown in Ref.31 for visible light, and explainedin Fig. 2b. The fact that we also observe asixfold pattern strongly suggest that our THzphotoresponse is dominated by the PTE effect.To further confirm that the PTE mechanismdominates over alternative photocurrent mech-anisms, such as bolometric and photogatingeffects, we measured the photocurrent as a func-tion of bias voltage applied between the sourceand drain contacts. The drain current increases

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Figure 2: a) Photoresponse as a function of voltages applied to the two antenna branches/gates, with radiationat 2.52 THz. We use our THz gas laser with an average incident power of Pin = 5 mW, and a peak irradiancein the center of the focus of 1.8·104 W/m2. The THz light is polarized parallel to the antenna axis. The sixfoldpattern, as in Refs.,29,31 indicates that the photoresponse is generated through the PTE effect. The photoresponseis the photocurrent normalized by the power in a diffraction-limited spot, i.e. the responsivity R. The maximumresponsivity occurs in the pn- and np-regions. b) Line cut at the location of the dashed line in panel a, showinga double sign change (red dots and line; left vertical axis) as a function of carrier density (controlled through gatevoltage VL). The blue line represents the Seebeck coefficient (calculated from the experimentally obtained graphenemobility, see SI; right vertical axis). The double sign change occurs due to the non-monotonous dependence of theSeebeck coefficient on carrier density: for a constant Seebeck coefficient in one region (dashed horizontal line), theSeebeck coefficient of the other region is first higher, then lower and then again higher, giving rise to two sign changes,as indeed observed experimentally. c) The extracted Johnson noise current, calculated from the resistance that wasmeasured simultaneously with the result in panel a. d) The noise-equivalent power (NEP), extracted from theresults in panels a and c, normalized to a diffraction-limited spot. The white cross indicates the gate configurationthat corresponds to the lowest NEP: the left (right) gate at 0.20 V (-0.72 V), corresponding to an electron densityof 7.5·1011 cm−2, EF = +100 meV (hole density of 3.6·1011 cm−2, EF = −70 meV).

linearly with applied bias voltage, whereas thephotocurrent remains constant (see SI), in con-tradiction with what is expected for the bolo-metric and photogating effects. Thus, theseresults show that the photo-thermoelectric ef-fect is responsible for the observed THz pho-toresponse. We find the largest photoresponsein the pn-junction and np-junction regimes, asexpected, relatively close to the Dirac point.

We now proceed with quantifying the sen-sitivity of our THz photodetector. First, weidentify the largest responsivity R = IPTE/Pdiff

at the optimal gate configuration for Device A.We note that the responsivity that we use isthe responsivity normalized by the power in adiffraction-limited spot with NA = 1. In someof the literature, a responsivity is provided that

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is normalized by the amount of power that isactually incident in the experiment Pin. How-ever in the case where the wavelength is largerthan the photodetector device this number doesnot only depend on the device performance,but also on how well the THz light is focused.Alternatively, one can use the responsivity nor-malized to the power that is absorbed in theactual graphene channel or in the photoac-tive area, which would yield an artificially highnumber,32 as it is impossible to focus the THzlight in such a small area. Here we choose theresponsivity normalized by the incident powerin a diffraction-limited spot, because this is ar-guably the most technologically relevant num-ber (as this represents what will be reachedwhen combining the detector with an optimizedfocusing system, such as using a silicon hemi-spherical lens23–25), and it is the conventionthat is most commonly used in the literatureon THz photodetection (see also Table 1). Wecalculate the power in a diffraction-limited spotusing Pdiff = Pin · Adiff/Afocus, where Pin is themeasured total incident THz power, Adiff is thecalculated area of a diffraction-limited spot andAfocus is the measured area of the focused THzbeam. Typically, we have Adiff/Afocus ≈ 1/60(corresponding to a NA of ∼0.13 for our fo-cusing system based on a parabolic mirror, seeMethods for details). From Fig. 2a we extracta maximum responsivity of R = 14 mA/W (32V/W). For Device B, we find a maximum re-sponsivity value of R = 25 mA/W (105 V/W)(see Methods and SI). In both cases the THzlight was at 2.52 THz (corresponding to a wave-length of 118.96 µm, 84 cm−1).

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Figure 3: a) Photocurrent as a function of THz laserpower (in a diffraction-limited spot) Pdiff in log-logscale. All round data points correspond to Device A,whereas the light blue squares correspond to Device B.The lines through the experimental data points are fitsaccording to IPTE ∝ P γdiff . The obtained exponent isclose to 1 for all data sets. For Device A, these datacorrespond to a gate configuration of VL = 0 V andVR = -0.67 V, corresponding to an electron (hole) den-sity of 4.2·1011 (-2.7·1011) cm−2. b) Responsivity Ras a function of THz wavelength (red dots, left verticalaxis), with the same (sub-optimal) gate configuration asin panel a. The black line (right vertical axis) shows theresult for the antenna-induced absorption enhancementin the graphene channel. The red dashed line illustratesthe trend of the experimental points. c) Results of thepulsed laser experiment, where the photocurrent wasamplified by a fast current pre-amplifer (Femto) and thedata were acquired with a fast oscilloscope. The insetshows how the photovoltage VPTE follows the switchingof the pulsed laser. The red and blue (plotted with anoffset) open dots show the obtained photovoltage in asmall time window marked in the inset, with the blackline giving the result of exponential fits with timescalesof 40 (24) ns for the red (blue) curve.

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Using the extracted responsivity, we now de-termine the sensitivity of the detector. For this,we note that our detector operates without bias,which means that it is limited by the Johnson

or thermal noise, given by: Inoise =√

4kBT∆fR

.

Here, kB is the Boltzmann constant, T is thetemperature of operation, ∆f is the spectralbandwidth and R the resistance. We show theJohnson noise current of Device A as a functionof the two gates voltages in Fig. 2c, calculatedfrom the measured resistance R. The resis-tance was measured simultaneously with thephotoresponse in Fig. 2a, which we used todetermine the responsivity R. As expected,we see that a higher noise current occurs forlower resistance values (away from the Diracpoint), whereas we obtain lower noise valuescloser to the Dirac point, where the grapheneresistance is higher. The photodetection sen-sitivity is given by NEP= Inoise/R, which weshow as a function of the two gate voltages inFig. 2d. The lowest values for the NEP occurat the pn- and np-regions close to the Diracpoint, where the responsivity is highest andthe noise is lowest. The lowest value of theNEP map was 200 pW/

√Hz for Device A and

80 pW/√

Hz for Device B (see Methods and SI).

An important characteristic of an ideal THzdetector is having a large range of powers overwhich the response is linear, i.e. a large dynamicrange. Thus, we measure the photocurrent vs.Pdiff for four different THz frequencies as shownin Fig. 3a. We vary the THz power over morethan 3 orders of magnitude (using the THzgas laser setup), and fit the data with a simplepower law IPTE ∝ P γ

diff . We obtain for Device Aat 2.5 THz a power of γ = 1.1±0.2 and for De-vice B γ = 1.1±0.15 (95% confidence intervals).This shows that the photoresponse depends lin-early on the THz power over a range of morethan three orders of magnitude. The reason forthe linear photoresponse as a function of poweris the fact that the photodetector operates inthe weak heating regime, where ∆T Tambient,i.e. the change in temperature of the electronicsystem is smaller than the ambient tempera-ture Tambient. When ∆T approaches Tambient, we

expect a sub-linear dependence of photocurrenton power, with an exponent that tends to γ =0.5.

Regarding the range of frequencies where ourdetectors operate, we note that this is onlylimited by the antenna structure. The rea-son behind the spectrally ultra-broad photore-sponse of graphene is the efficient heating ofthe electrons, which occurs irrespective of thewavelength of the incident light, i.e. whetherintraband or interband light absorption oc-curs.28,35 We characterize the spectral responseof our detector by measuring the responsivity,while varying the frequency from 1.83 to 4.25THz (see Fig. 3b). We observe a trend wherethe responsivity peaks around 3 THz. Thiscorresponds reasonably well with the antennabeing optimized for a frequency of 2 THz usingfull wave simulations (see Methods and Fig.3b). The discrepancy likely comes from thefact that a simplified structure was simulated,which didn’t contain all the metallic parts thatthe actual device has. Importantly, these re-sults confirm that the spectral range where theTHz detector operates is currently limited onlyby the antenna. Thus, using more spectrallybroad antennas or a combination of antennasone could extend the spectral range of our pho-todetector, covering the spectrum all the wayfrom the ultraviolet, through the visible andinfrared to the terahertz.

In the following, we discuss the speed of ourPTE THz photodetector. We analyze the speedin Fig. 3c, where we rapidly switch the THz ra-diation on (white) and off (yellow) using ourpulsed THz QCL (see Methods). We observethat the photoresponse of our detector VPTE

closely follows the laser switching behavior.We quantify the detector speed by fitting theVPTE rise and fall dynamics (see also SI) withsimple exponential equations, and obtain anexponential (1/e) response time of 32±11 ns,corresponding to a bandwidth of ∼5 MHz. Inthis measurement, the speed is most likely lim-ited by the measurement electronics, namelyby the 3.5 MHz bandwidth of the current pre-amplifier, rather than by the PTE THz detector

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itself. Indeed, the intrinsic speed of the detec-tor is expected to be significantly higher, sinceultimately the intrinsic response time is limitedby the RC-time of the detector. Performingthis calculation (see Methods), we obtain a risetime of 56 ps, corresponding to a detectionrate of 6 GHz for our device with a mobility of20,000 cm2/Vs. For a device with a mobilityof 100,000 cm2/Vs (see SI), we find 9 ps, cor-responding to 40 GHz. Thus, extremely fastTHz photodetection with switching times inthe picosecond range should be possible.

We now discuss more of the underlyingphysics of the PTE detector, using a simple an-alytical model that provides the rationale be-hind our detector design. Owing to the differ-ence in Seebeck coefficients at the pn-junction,a local photo-thermoelectric voltage is created,which leads to the flow of a photocurrent be-tween the source and drain contacts that areconnected to the graphene channel. The PTEphotocurrent is then given by29

IPTE =(S1 − S2) ∆T

R, (1)

where S1 and S2 are the Seebeck coefficients(also called thermopower) of the two regions ofthe graphene channel that are independentlycontrolled by the gates/antenna branches, ∆Tis the temperature increase of the electronicsystem induced by THz radiation, and R is thetotal electrical resistance, accounting for thegraphene and contact resistances. It is worthmentioning that this current is generated underzero applied source-drain bias voltage, resultingin very low detector noise (Johnson noise) andextremely low power consumption.

Graphene is an ideal material to exploit thePTE effect for THz detection, because theterm (S1 − S2) ∆T can be large and R is typi-cally small, in particular for high-quality, hBN-encapsulated graphene. The Seebeck coefficientof graphene is intrinsically quite large, on theorder of 100 µV/K36 and S1 and S2 are inde-pendently tunable through the gates, meaningthat (S1−S2) can be maximized. Furthermore,

∆T can be large in graphene (up to severalthousand K), because of efficient heating ofthe electrons after absorbing THz light, dueto strong electron-electron interactions, andbecause the hot carriers are relatively weaklycoupled to the crystal lattice.28

Our photodetector design maximizes the PTETHz photoresponse, particularly by maximiz-ing ∆T and minimizing R. From a simple heatequation, the temperature increase ∆T (aver-aged over all charge carriers in the photoactivearea) is given by

∆T ≈ Pabs

AactiveΓcool

(2)

where Pabs is the amount of THz power thatis absorbed in the active area of the graphenechannel and Γcool is the heat conductivity thatdescribes the coupling of the heated electronsystems to its environment. The photoactivearea is given by Aactive = 2`cool · w, where `cool

is the hot-carrier cooling length, which can beseen as the length scale over which hot car-riers can move before cooling down (typically0.5 – 1 µm at room temperature,29,31,35,37,38 seealso Fig. 1c). In the case of hBN-encapsulatedgraphene, Γcool is the out-of-plane, interfacialheat conductivity where hot graphene carrierscouple to hyperbolic hBN phonons.37 We opti-mize ∆T by maximizing Pabs and minimizingAactive. We maximize the amount of absorbedTHz power Pabs by using a dipole antenna witha narrow gap, which focuses the incoming THzradiation down to the small (compared to theTHz radiation wavelength) graphene photoac-tive region. We further maximize ∆T by usinga narrow channel width w of 2 µm. Basically,the smaller the area where the incident poweris absorbed, the smaller the amount of elec-trons that will share the heat, and thereforethe larger the increase in temperature of theelectronic system, ∆T .

In order to further increase the responsivity,we reduce the overall resistance R of the device,and optimize the shape of the graphene chan-nel. We achieve low R by using high-qualityhBN-encapsulated graphene (see Fig. 1b).39,40

9

Page 10: Fast and sensitive terahertz detection using an antenna

This method enables mobility values as highas 100,000 cm2/Vs at room temperature, andlow levels of intrinsic doping (see SI). We fur-thermore pattern the graphene channel in an“H-shape” (see Fig. 1a), in order to reducethe overall device resistance R. This shape iscrucial because it has a small width w in thecentral part of the channel – ensuring smallAactive and thus large ∆T – while having alarger width towards the contacts – minimizingthe graphene sheet resistance. Furthermore,the large interface with the source and draincontacts minimizes the contribution of contactresistance to the overall resistance R. We as-sess the validity of the analytical model of Eqs.1-2, by comparing the results with numericalsimulations of the PTE photocurrent gener-ated in different graphene geometries (see SI).We find agreement between the analytical andnumerical results, showing the validity of ouranalytical approach. Importantly, the analyti-cal model gives us insights into the physics thatdetermines the detector response, thus allowingfor optimization strategies. The advantage ofthe numerical simulations is that they are alsovalid for non-rectangular graphene shapes. Ourdetector design is the result of these analyticaland numerical simulations.

Based on the analytical model for the PTEresponse, we now examine our experimentalresults quantitatively. We have measured aphotocurrent of IPTE = 1.14 µA (Device A, 2.5THz) for an incident power of Pin = 5 mW (fo-cused to a spot size Afocus, see Methods). UsingEq. 1 with (S1 − S2) = 160 µV/K (estimatedfrom Ref.41) and R = 2.3 kΩ (measured), wefind an experimental temperature increase of∼16 K (confirming the weak heating regime).Then using Eq. 2 with interfacial heat con-ductivity Γcool = 7·104 W/m2K (determined inRef.37), cooling length `cool = 510 nm (from themobility and interfacial heat conductivity, seeSI), and channel width w = 2 µm (measured),we find the absorbed power (in the active areaof the graphene channel) to be Pabs = 2.3µW. We compare this value with the absorbedpower we find from numerical simulations of theantenna-graphene structure, using the same ir-

radiance as in the experiment (see Methods).These simulations give an absorbed power (inthe entire graphene channel) of Pabs,sim = 7µW (at 2.5 THz). This number is close to thenumber we obtained experimentally, addingcredibility to our assignment of the PTE as thedominant photoresponse mechanism and to thevalidity of our analytical model. We ascribe thelower experimental value (by a factor ∼3) tonon-optimal performance of the actual antennain the photodetector device, most likely dueto the presence of metallic regions around theantenna (see SI). Furthermore, the simulationsconsider the absorption in the entire graphenesheet, rather than only in the photoactive areaof the graphene channel. Notably, we point outthat without the antenna, the amount of inci-dent THz light from a diffraction-limited spotthat would be absorbed in the photoactive areaof the graphene channel would be more thanthree orders of magnitude lower, highlightingthe importance of the antenna-integration. Weillustrate this in Fig. 3b, where we show theantenna-induced absorption enhancement, de-

fined as G =Pabs,sim,w/ antenna

Pabs,sim,w/o antenna. These simulations

show that the antenna enhances the grapheneabsorption by more than three orders of mag-nitude.

Finally, we compare the performance of ourphotodetector with respect to other graphene-based THz photodetectors in the literature.We first compare with other detectors wherethe photodetection mechanism was explicitlyascribed to the PTE effect (see Table 1). Sincenot every report used the same power normal-ization procedure for the responsivity and NEP,we mention explicitly the normalization proce-dure that was used. We note that our THzdetector is 2–4 orders of magnitude more sen-sitive than any other THz PTE photodetector(if the same normalization procedure would beapplied). We attribute this to our novel designwith the antenna/gating structure, the opti-mal graphene channel geometry and the useof high-mobility hBN-encapsulated graphene.Furthermore, the sensitivity that we obtain isvery similar to, or better than, the most sen-

10

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Table 1: Comparison of graphene-based THz photodetectors.

Reference Mechanism NEP Normalization Speed Freq. range

(pW/√

Hz) area Anorma (ns) (THz)

This work PTE 80 λ2/π <30 1.8 – 4.2532 PTE 1100 ∼ λ2/3350 0.11 2.533 PTE 350 ∼ λ2/450 9000 0.08 – 0.324 Rectification 130 none - 0.422 Plasma waves 2000 λ2/4 - 0.29 – 0.3825 PTE/plasma waves 600 noneb - 0.13 – 0.4526 Ballistic rectification 34 λ2/4π - 0.07-0.69

a The normalization area Anorm refers to the area to which the incident power was normalized: Pnorm = Pin ·Anorm/Afocus. In our work, for example, we use the power in a diffraction-limited spot Pdiff = Pin · Adiff/Afocus,i.e. we use Anorm = Adiff = λ2/π.b Whereas the incident power was not normalized to any area, a correction of the incident power was applied toaccount for losses occurring in the focusing system.

sitive graphene-based THz detectors reportedin the literature.24,26 The operation of thosedetectors, however, has only been shown forfrequencies below 1 THz and no response timeshave been measured. Additionally, it’s impor-tant to point out that the Drude optical con-ductivity and therefore absorption in grapheneis higher in the GHz range than in THz,42,43

hence a direct comparison with detectors oper-ating below 1 THz is not straightforward sincewe do not normalize the detector responsivityby the graphene absorption.

In conclusion, we have demonstrated a novelTHz photodetector, which is dominated bythe photo-thermoelectric effect. It operates atroom temperature, is highly sensitive and veryfast, has a wide dynamic range and operatesover a broad range of THz frequencies. We haveoptimized the PTE THz detector by using asplit-gate/antenna structure with narrow gap,which funnels the incident THz light exactlyat the small photoactive area of the detectorleading to strongly enhanced THz absorptionin graphene. This structure simultaneouslyallows for tuning the detector to the optimalgating configuration, where a pn-junction iscreated in the graphene channel. Furthermore,we have used an “H-shaped”, high-quality,hBN-encapsulated graphene channel with anarrow width, in order to have a small photo-

active area, thus achieving a large THz-inducedchange in temperature, and a low overall deviceresistance.

Given the qualitative and quantitative under-standing we have developed of the performanceof our detector, we identify strategies for furtherimproving its performance. Most importantly,by optimizing the antenna, a higher absorp-tion and therefore lower NEP can be achieved.Additionally, by using a more broadband an-tenna, the detector will be sensitive for a largerrange of THz frequencies. The sensitivity canbe further enhanced by having a lower ther-mal conductivity Γcool. This could be achievedby exploring alternative encapsulation materi-als, rather than hBN, e.g. a transition metaldichalcogenide (TMD) material, and by oper-ating at a lower temperature. We estimate thatit will be possible to reach an NEP in the lowpW/

√Hz-regime. We expect that the unique

combination of high sensitivity and fast opera-tion means that these THz PTE detectors willplay an important role in a large spectrum ofapplications.

Supporting Information

Raman, electrical characterization and opticalimages of the devices, fall time measurements of

11

Page 12: Fast and sensitive terahertz detection using an antenna

device A, power dependence and scanning pho-tocurrent measurements of device B and ther-moelectric simulations.

Methods

Sample fabrication

First we patterned the antenna/gate structureon transparent SiO2 (Infrasil) substrate usingelectron beam lithography followed by evapo-ration of titanium (2 nm) / gold (30 nm). Theantenna gap was 200 nm (100 nm) for device A(B). We then released an hBN/graphene/hBNstack onto the antenna/gate structure. Thestack elements (top and bottom hBN andgraphene) were mechanically cleaved and exfo-liated onto freshly cleaned Si/SiO2 substrates.The full stack was prepared by the Van derWaals assembly technique39,40 and releasedonto the antenna/gate structure. This wasfollowed by patterning source and drain elec-trodes, using electron beam lithography with aPMMA 950 K resist film and exposing it to aplasma of CHF3/O2 gases for partially etchingthe stack. Consequently, we evaporate side con-tacts of chromium (5 nm) / gold (60 nm) andlift off in acetone as described in Ref.39. Finally,the encapsulated graphene was etched into the“H” shape using a plasma of CHF3/O2 gases.From gate-dependent measurements (varyingVL and VR simultaneously) on Device A, we ex-tract a mobility >20,000 cm2/Vs and a contactresistance of 126 Ω (3.8 kΩ · µm) (see SI).

Measurements

In one setup (used for all Figs. except for Figs.1d and 3c), we used a continuous wave THzbeam from a gas laser (FIRL 100 from Edin-burgh Instruments) providing a maximum out-put power in the range of a few tens of milli-watts, and frequencies of 1.83, 2.52, 3.11 and4.25 THz. The device position was scanned us-ing a motorized xyz-stage. The THz laser wasmodulated at 266 Hz using an optical chop-per and the photocurrent was measured us-ing a lock-in amplifier (Stanford). We verifiedthat the output THz beam was strongly po-

larized (only 2% of residual unpolarized light)and mounted the detector with the antenna axisparallel to the polarization. The THz light wasfocused using a gold parabolic mirror with focaldistance 5 cm. The THz power was measuredusing a pyroelectric THz detector from Gentec-EO placed at the sample position. The sec-ond setup (used for Fig. 1d and 3c) contained apulsed QCL at 3.4 THz, with an expected risetime <1 ns.

Responsivity calculation

For the responsivity R = IPTE/Pdiff , we ex-tracted the PTE photocurrent IPTE from theoutput signal of the lock-in amplifier VLIA us-ing IPTE = 2π

√2

4GVLIA,20,22 where G is the gain

factor in V/A (given by the lock-in amplifier).The power in a diffraction-limited beam is givenby Pdiff = Pin · Adiff/Afocus, where the ratio

Adiff/Afocus =w2

0,diff

w0,xw0,y. In order to obtain w0,x

and w0,y we use our observation that the pho-toresponse is linear in laser power and mea-sured the photocurrent while scanning the de-vice in the x− and y−direction. The photocur-rent is then described by Gaussian distributions∝ e−2x2/w2

0,x and ∝ e−2y2/w20,y , where w0,x and

w0,y are the respectively obtained spot sizes (re-lated to the standard deviation via σ = w0/2and to the FWHM via FWHM =

√2 ln(2)w0).

For Device A, we obtained w0,x = 263.3 µm andw0,y = 331.2 µm. For the diffraction-limitedspot, we took w0,diff = λ

π, with λ the THz laser

wavelength. The diffraction-limited area is thustaken as Adiff = πw2

0,diff = λ2/π.

Antenna simulations

The full wave simulations were performed inComsol. The frequency dependent permittiv-ity of hBN was taken from Ref.44. The op-tical conductivity of graphene was calculatedemploying the local random phase approxima-tion at T = 300 K with a scattering time of100 fs. In the simulations, for simplicity, theFermi energy of the graphene sheet was spa-tially constant. A plane wave source was usedfor illumination, where the incident power wasnormalized to give the same irradiance as the

12

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experiment.

Speed calculations

The electrically-limited operation frequency ofthe detector is related to the RC-time con-stant τ = RC, with R total graphene resis-tance (including contact resistance), and C to-tal graphene capacitance. The operating speedis then given by the rate f = (2πτ)−1. The risetime τrise is the measure of the photodetector re-sponse speed to a stepped light input signal. Itis the time required for the photodetector to in-crease its output signal from 10% to 90% of thefinal steady-state output level. The rise time iscalculated as τrise = τ · ln(9) = (2πf)−1 · ln(9)= 0.35/f .

Acknowledgments

The authors thank Mark Lundeberg and Ia-copo Torre for fruitful discussions. F.H.L.K.acknowledges financial support from the Span-ish Ministry of Economy and Competitive-ness, through the Severo Ochoa Programmefor Centres of Excellence in R&D (SEV-2015-0522), support by Fundacio Cellex Barcelona,Generalitat de Catalunya through the CERCAprogram, and the Agency for Managementof University and Research Grants (AGAUR)2017 SGR 1656. Furthermore, the researchleading to these results has received fundingfrom the European Union Seventh FrameworkProgramme under grant agreement no.785219Graphene Flagship (Core2). ICN2 is supportedby the Severo Ochoa program from SpanishMINECO (Grant No. SEV-2017-0706). K.-J.T.acknowledges support from a Mineco YoungInvestigator Grant (FIS2014-59639-JIN). S.C.acknowledges funding from the Barcelona In-stitute of Science and Technology (BIST), theSecretaria dUniversitats i Recerca del Depar-tament dEconomia i Coneixement de la Gen-eralitat de Catalunya and the European So-cial Fund FEDER. M.S.V. acknowledges fi-nancial support from the ERC Project 681379(SPRINT) and partial support from the secondhalf of the Balzan Prize 2016 in applied photon-ics delivered to Federico Capasso. A.Y.N. ac-

knowledges funding from the Spanish Ministryof Economy, Industry and Competitiveness, na-tional project MAT2017-88358-C3-3-R.

13

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Supporting Information

1) Thermoelectric simulations

To calculate the PTE response of our device we solved numerically the linearized thermoelectricequations:45

jQ(r) = −σ(r)∇V (r)− σ(r)S(r)∇T (r), (3)

jE(r) = −Π(r)σ(r)∇V (r)− [κ(r) + Π(r)σ(r)S(r)]∇T (r), (4)

where jQ(r), jE(r) are the electric and energy current density respectively, V (r) is the voltage,T (r) is the local temperature, σ(r) is the electrical conductivity, S(r) is the Seebeck coefficient,Π(r) is the Peltier coefficient, and κ(r) is thermal conductivity. These two equations are coupledto the continuity equations for the charge and energy currents:

∇ · jQ(r) = 0, (5)

∇ · jE(r) = −g(r)[T (r)− T0] + JE(r). (6)

Here g(r) parametrizes the thermal conduction to the substrate,37 T0 is the substrate temperature,and JE(r) is a local heat source, that in our case is due to light absorption. We solved these equa-tions inside a 2D simulation box [0, Ltot]× [0,Wtot] illustrated in Fig. S5 that includes the graphenesheet and the gold contacts. We artificially included a small rectangular region of dimension δ×Wbetween the graphene and the gold contacts to account for finite contact resistance by choosing thevalue of its conductivity σ = δ/Rcont with Rcont being the value of the gold-graphene contact resis-tance. We assumed that the material parameters σ(r), S(r), Π(r), κ(r), and g(r) are piecewiseconstant in the regions described in Fig. S5. Since, because of Onsager relations, Π(r) = T0S(r),and the thermal conductivity is related to the electrical conductivity by the Wiedemann-Franz lawκ(r) = L0σ(r)T0, with L0 ≡ π2k2

B/(3e2) = 2.44 · 10−8WΩK−2, we have only three independent

parameters (σ(r), S(r), g(r)) that are listed in table S1.Eqs. (3,4,5,6) need to be supplemented with boundary conditions (BCs). We used Dirichlet BCs

at x = 0, Ltot. These read:

V (x = 0, y) = Vsd, (7)

V (x = Ltot, y) = 0, (8)

T (x = 0, y) = T (x = Ltot, y) = T0. (9)

We assumed instead homogeneous Neumann condition on the remaining part of the boundary

n · jQ(r) = 0, (10)

n · jE(r) = 0, (11)

n being the outward normal unit vector. We solved numerically Eqs. (3,4,5,6), with BCs (7,11)using the Finite Volume Method (FVM) on a regular square grid of 400x240 cells. Once the solutionis found, the current flowing in the device can be calculated as

I ≡∫ Wtot

0

Jx(0, y)dy =

∫ Wtot

0

Jx(Ltot, y)dy =Vsd

R+ IPTE, (12)

where the last equality holds because of linearity, R is the resistance, and

14

Page 15: Fast and sensitive terahertz detection using an antenna

IPTE =

∫drRint(r)JE(r). (13)

To find R we simply calculate the current by setting JE(r) = 0. The responsivity Rint(r0) ata given position r0 is instead calculated by setting Vsd = 0 and JE = δ(r − r0), and calculatingthe corresponding current. This step is repeated for every r0 in the simulation grid to obtain theresponsivity maps in Fig. S5.

Table S1: Material parameters

Material σ[S] S[µV/K] Γcool[W/m2K]

Graphene n (p) doped 1.3·10−3 a 80 (-80)41 7·104 37

Gold 4b 0c 300·104 46,47

Interface contact 2.5·10−6 d 0c 100·104

a When considering EF = 50 (-50) meV, T = 300 K and 200 fs relaxation timefor both doping type n (p). b For 100 nm gold. c We neglect the contributionof the Seebeck coefficient of the metal. d For a δ = 25 nm.

15

Page 16: Fast and sensitive terahertz detection using an antenna

2) Supplementary figures

a

60 μm

b

c d

4 μm300 μm

4 μm

Figure S1: Optical microscope images of the graphene-based THz photodetectors. a) 10x magnifica-tion image of Device A, showing the metallic rods contacting the antenna branches and source-drainelectrodes. b) 100x magnification image of Device A, displaying the area of the photodetector con-taining the antenna/gate structure, source-drain electrodes and “H-shaped”, h-BN encapsulatedgraphene. c) 5x magnification image of Device B and d) 100x magnification image of Device B.

16

Page 17: Fast and sensitive terahertz detection using an antenna

Figure S2: a) Measured resistance map as a function of the right gate (left axis) and left gate(bottom axis) for Device A. b) Resistance as a function of graphene charge carrier density (linecutin dashed line shown in a)). We fit the resistance R curve using the model from Ref.48, whereR = Rc + (L/w)(µen)−1, Rc is contact resistance, L is channel length, w is channel width, µ ismobility, e is elementary charge, and the carrier density is given by n =

√(n∗)2 + (β(Vg − VDirac))2.

Here n∗ is the residual doping concentration, Vg is gate voltage, VDirac is the gate voltage thatcorresponds to the Dirac point, and β = ε0εhBN/dhBNe, where ε0 is vacuum permittivity, εhBN thedielectric constant of hBN and dhBN the thickness of the bottom hBN. We obtained 22,000 and19,000 cm2/Vs for electron (red) and hole (blue) mobility, respectively. We extracted a contactresistance of Rc = 126 Ω (3.8 kΩ · µm), and a residual doping concentration of n∗ = 1.6·1011 cm−2.c) Carrier mobility as a function of graphene charge carrier density extracted from the conductancemeasurement,39 where blue (red) corresponds to hole (electron) mobility.

Figure S3: Raman spectroscopy measurements of Device A. a) Histogram plot of the full-width-half-maximum of the graphene 2D peak (Γ2D) across the ∼15x15 µm2 region marked in red on theoptical picture (see inset). The white scale bar corresponds to 30 µm. The inset shows a typicalRaman spectrum of the monolayer graphene. The mean Γ2D is ∼17.5 cm−1, characteristic of highquality single layer graphene.49 b) 2D-peak versus G-peak frequency (ω2D and ωG, respectively)extracted from the same Raman map as in panel a. The colorbar represents the Γ2D of the recordedspectrum. The data shows low doping, as confirmed in transport measurements (see Fig. S2), andmoderate levels of strain.49

17

Page 18: Fast and sensitive terahertz detection using an antenna

Figure S4: Characterization of the Hall bar reference device fabricated following the same procedureas the photodetector (see Methods). a) Optical image of the initial hBN/graphene/hBN stack. b)Optical image shown in panel a with enhanced contrast. The graphene flake is optically visible(compare the graphene shape with the Raman map shown in the inset of panel c). c) Histogramplot of the Raman scan (see inset) showing the full-width-half-maximum of the graphene 2D Ramanpeak (Γ2D). The mean Γ2D is ∼ 18.1 cm−1, characteristic of high quality single layer graphene. d)Scattering plot of the 2D-peak versus the G-peak frequency (ω2D and ωG, respectively), where thecolorbar represents the Γ2D of the recorded spectrum (inset of panel c). The Raman data showscomparable behavior as the photodetector (see Fig. S3b) with low Γ2D, low doping and moderatelevels of strain.49 e) Resistance as a function of the charge carrier density of the measured Hallbar device (see inset). We fit the resistance R curve using the model from Ref.48, and obtained103,000 and 96,000 cm2/Vs for the electron (red) and hole (blue) mobilities, respectively. f) Carriermobility as a function of the charge carrier density extracted from the conductance measurement39,where blue (red) corresponds to hole (electron) mobility. These results show that a mobility of100,000 cm2/Vs for these kind of photodetector devices is realistic, and therefore a detection speedin the 10 ps-range can be achieved.

18

Page 19: Fast and sensitive terahertz detection using an antenna

0.12

0.06

0.0

-0.06

-0.12

R = 3.8 kΩ

int,sim_max = 0.126 A/W

int,sim_tot = 0.040 A/W

NEP = 52.2 pW/ Hz

a b c

d e f

R = 22.2 kΩ

int,sim_max = 0.130 A/W

int,sim_tot = 0.043 A/W

NEP = 20.1 pW/ Hz

R = 5.3 kΩ

int,sim_max = 0.542 A/W

int,sim_tot = 0.48 A/W

NEP = 3.7 pW/ Hz

in

t,si

m[A

/W]

in

t,si

m[A

/W]

in

t,si

m[A

/W]0.12

0.06

0.0

-0.06

-0.12

0.45

0.150.0

-0.15

-0.45

Lsd = 3.6 µm

w =

6 µ

m

3.6 µm 3.6 µm

6 µm1 µm1 µm

Ltot

Graphene (p doped)

Graphene (n doped)

MetalInterface contact

Wto

t

Figure S5: Thermoelectric simulations results,50 as in Fig. 1c, which represent the resulting pho-toresponse after local photoexcitation, expressed in photocurrent normalized by absorbed power,i.e. internal responsivity (Rint,sim as defined in Eq. S11, where JE(r) represents the locally absorbedpower). These simulations were based on similar characteristics of the measured samples, with agraphene scattering time of 200 fs (mobility 20,000 cm2/Vs), contact resistance of 10 kΩ·µm, 3.6 µmof source-drain distance (Lsd), Γcool = 7·104 W/m2K, EF = 50 meV and -50 meV for n- and p-dopedgraphene regions respectively. Panels a-c) show the simulated device geometries and panels d-f)the internal responsivity (Rint,sim) calculated at each position across the device. The R, Rint,sim max,Rint,sim tot and NEP below panels d-f) indicate total device resistance (including graphene sheetand contact resistance), the maximum internal responsivity generated at the pn junction, totalinternal responsivity (which takes into account also the opposite sign responsivity generated at themetal-graphene interface, i.e. Rint,sim tot = Rint,sim max− | Rint,sim min |) and noise-equivalent power,respectively. The simulations show that decreasing the width of the graphene channel (going fromthe design of panel a to the design of panel b) does not lead to any change in responsivity, but adecrease in noise-equivalent power. The responsivity is constant because of the trade-off betweenthe increased ∆T due to the smaller active area and the increased device resistance due to thesmaller width. The NEP is reduced, because the higher device resistance leads to reduced thermalnoise. Then, by using the design with an “H-shaped” graphene channel in panel c, we both increaseresponsivity and decrease NEP. The main reason is that the active area is significantly reduced,without increasing too much the device resistance. Furthermore, the maximum responsivity andtotal internal responsivity are now very similar, because the PTE response at the pn-junction dom-inates. Therefore, this is the preferred design. We compare the simulation results for the internalresponsivity Rint,sim with the analytically obtained values (Rint,analyt) using the equations in themain text and the device resistances obtained from these simulations, and obtain Rint,analyt = 0.12,0.13 and 0.55 A/W for the designs from panels a), b) and c) respectively. These analytical valuesare in excellent agreement with the Rint,sim max values obtained from simulations.

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-0.6

-0.4

-0.2

0.0

200150100500

-0.4VPTE[V]

-0.6

-0.2

0.0

0

Time [ns]50 100 150 200

Figure S6: Results of the pulsed laser experiment, showing the fall time corresponding to the tworegions (red and blue, the latter one plotted with an offset) of the inset of Fig. 3c of the main text.The open dots show the acquired photovoltage and the black lines represent the fit results with theexponential fits. We obtain an exponential fall time of 47 (28) ns for the red (blue) curve. As inthe case of the rise time determination in the main text, this timescale is limited by the currentamplifier with a bandwidth of 3.5 MHz.

3.0

2.5

2.0

1.5

1.0

0.5

Drain current (µA

)

1086420Bias voltage (mV)

-50x10-9

-40

-30

-20

-10

0

Phot

ocur

rent

(A)

b

0 2 4 6 8 10

SD bias [mV]

50

I PTE[nA] 40

30

20

10

0

I D[µA]

2.0

1.5

1.0

0.5

2.5

3.0

Figure S7: Photocurrent and drain current measured simultaneously as a function of applied biasvoltage between the source and drain contacts. We notice a linear increase of the drain currentwhile increasing the bias, whereas the photocurrent remains constant.

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10-8

2

4

6

10-7

2

4

6

10-6

6 8

10-6

2 4 6 8

10-5

2 4 6

140x10-9

120

100

80

60

40

20

0

Photo

curr

ent

(A)

3.02.52.01.51.00.50.0Position (mm)

a

0 0.5 1.0 1.5 2.0 2.5

Position [mm]

140

I PTE[nA]

100

60

0

20

b

Pdiff [µW]

I PTE[nA]

1000

10110

100

3.0

Figure S8: Characterization of Device B. a) Photocurrent generated as a function of the scanposition of the device. The red circles correspond to the experimental points and the red lineto the Gaussian distribution fit. We obtain a beam focus FWHM of 897 µm at 2.52 THz. Weobserve a maximum IPTE of 136 nA for an incident power (Pin) of 2.88 mW (Pdiff = Pin ·Adiff/Afocus

= 7.1 µW). Thus, the responsivity is R = IPTE/Pdiff = 19 mA/W (80.4 V/W). The sample waselectrostatically doped with the left (n-doped, 60 meV) and right gate (p-doped, 50 meV) forminga pn-junction. b) Photocurrent as a function of incident power. It shows a linear trend over threeorders of magnitude according to the fit displayed in dashed line. The maximum responsivity wasR = 25 mA/W (105 V/W), from a photocurrent of IPTE = 145 nA, for an incident power of Pin =2.28 mW (Pdiff = 5.6 µW, for the same beam focus at 2.5 THz and pn-junction configuration as inpanel a). Using this responsivity and the Johnson noise that corresponds to the 4.2 kΩ measureddevice resistance, we find an NEP of 80 pW/

√Hz.

40

30

20

10

0

x10

3

-40 -20 0 20 40x10

-6

500x10-6

400

300

200

100

0

PC

15.014.514.013.513.0Position (mm)

PC PC#1

200

a

Position [mm]0.5

I PT

E[n

A]

400

1.0

0

1.50.0

X dir.

2.0

Position [μm]20 0 20-40 40

I PT

E[a

.u.]

b

Y dir.

0

10

20

30

40

FWHM

σ

w0

Figure S9: Characterization of spot size for measurements on Device A. a) Photocurrent as afunction of the scan position in x-direction (green) and y-direction (red) of the motorized stageonto which the device is mounted. The laser was tuned to 2.52 THz. The open dots represent theexperimental data and the lines the fits according to Gaussian distributions. We obtain a FWHMof 351 (348) µm for x- (y−) scan direction. b) Calculated Gaussian distribution representing adiffraction-limit focus at 2.52 THz. The arrows indicate the standard deviation σ, FWHM and spotsize w0, corresponding to 60, 50 and 13.5% of the maximum, respectively.

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a b c

int,sim[A/W

]

0.10

0.05

0.0

-0.05

-0.10

int,sim[A/W

]0.16

0.08

0.0

-0.08

-0.16 int,sim[A/W

]

0.32

0.16

0.0

-0.16

-0.32

b c

Figure S10: Thermoelectric simulations50, showing the internal responsivity (Rint,sim as defined inEq. S11, where JE(r) represents the locally absorbed power) for a fixed device geometry and threedifferent values of the interfacial heat conductivity Γcool. For all these three cases the device lengthand width dimensions are 10 and 6 µm respectively, EF = 50 meV (-50 meV) for n- (p-) doped regionand with a contact resistance of 10 kΩ ·µm. The Γcool is 7·104, 2·104 and 0.7·104 W/m2K for a), b)and c) respectively. As predicted from Eq. 2 in the main text, when decreasing Γcool, ∆T increasesand therefore Rint,analyt. In fact, by calculating the Rint,analyt = IPTE/Pabs = ∆S∆T

PabsR= ∆S

AactiveΓcoolR

as shown in the main text, we obtain excellent agreement between these calculations and thethermoelectric simulations values of Rint,sim for all three cases, namely Rint,analyt = 0.10, 0.19 and0.33 A/W for a), b) and c) respectively. These results show that the responsivity increases (andthe NEP decreases) with the square-root of the decrease in interfacial heat conductivity.

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References

(1) Tonouchi, M. Cutting-edge terahertz technology. Nature Photonics 2007, 1, 97–105.

(2) Ferguson, B.; Zhang, X.-C. Materials for terahertz science and technology. Nature Materials2002, 1, 26–33.

(3) Lee, M.; Wanke, M. C. Searching for a solid-state terahertz technology. Science 2007, 316,64–65.

(4) Mittleman, D. Sensing with Terahertz Radiation. Springer-Verlag: Berlin 2003, 342, 614–617.

(5) Appleby, R.; Wallace, H. B. Standoff detection of weapons and contraband in the 100 GHz to1 THz region. IEEE Trans. Antennas Propag. 2007, 55, 2944–2956.

(6) Federici, J. F.; Schulkin, B.; Huang, F.; Gary, D.; Barat, R.; Oliveira, F.; Zimdars, D. THzimaging and sensing for security applications - Explosives, weapons and drugs. SemiconductorScience and Technology 2005, 20, S266–S280.

(7) Siegel, P. H. Terahertz technology in biology and medicine. IEEE Transactions on MicrowaveTheory and Techniques 2004, 52, 2438–2447.

(8) Kleine-Ostmann, T.; Nagatsuma, T. A review on terahertz communications research. Journalof Infrared, Millimeter, and Terahertz Waves 2011, 32, 143–171.

(9) Ma, J.; Karl, N. J.; Bretin, S.; Ducournau, G.; Mittleman, D. M. Frequency-division multi-plexer and demultiplexer for terahertz wireless links. Nature Communications 2017, 8, 1–7.

(10) Mittendorff, M.; Shanshan Li,; Murphy, T. E. Graphene-Based Waveguide-Integrated Tera-hertz Modulator. ACS Photonics 2017, 4, 316–321.

(11) Gentec-EO, Pyroelectric terahertz detectors. 2018, available at http://www.gentec-eo.com/products/thz-detectors/ .

(12) Tydex, Golay cells terahertz detectors. 2018, available athttp://www.tydexoptics.com/products .

(13) Scontel, Superconducting Nanotechnology. 2018, available athttp://www.scontel.ru/terahertz/ .

(14) Sizov, F.; Rogalski, A. THz detectors. Progress in Quantum Electronics 2010, 34, 278–347.

(15) Virginia Diodes. Schottky diodes terahertz detectors. 2018, available athttp://www.vadiodes.com/en/products/detectors .

(16) Low, T.; Avouris, P. Graphene plasmonics for terahertz to mid-infrared applications. ACSNano 2014, 8, 1086–1101.

(17) Li, Z. Q.; Henriksen, E. A.; Jiang, Z.; Hao, Z.; Martin, M. C.; Kim, P.; Stormer, H. L.;Basov, D. N. Dirac charge dynamics in graphene by infrared spectroscopy. Nature Physics2008, 4, 532–535.

(18) Koppens, F. H. L.; Mueller, T.; Avouris, P.; Ferrari, A. C.; Vitiello, M. S.; Polini, M. Pho-todetectors based on graphene, other two-dimensional materials and hybrid systems. NatureNanotechnology 2014, 9, 780–793.

23

Page 24: Fast and sensitive terahertz detection using an antenna

(19) Bonaccorso, F.; Sun, Z.; Hasan, T.; Ferrari, A. C. Graphene photonics and optoelectronics.Nature Photonics 2010, 4, 611–622.

(20) Vicarelli, L.; Vitiello, M. S.; Coquillat, D.; Lombardo, A.; Ferrari, A. C.; Knap, W.; Polini, M.;Pellegrini, V.; Tredicucci, A. Graphene field-effect transistors as room-temperature terahertzdetectors. Nature Materials 2012, 11, 865–871.

(21) Mittendorff, M.; Winnerl, S.; Kamann, J.; Eroms, J.; Weiss, D.; Schneider, H.; Helm, M.Ultrafast graphene-based broadband THz detector. Applied Physics Letters 2013, 103, 21113.

(22) Spirito, D.; Coquillat, D.; De Bonis, S. L.; Lombardo, A.; Bruna, M.; Ferrari, A. C.; Pelle-grini, V.; Tredicucci, A.; Knap, W.; Vitiello, M. S. High performance bilayer-graphene Tera-hertz detectors. Applied Physics Letters 2014, 104, 061111.

(23) Zak, A.; Andersson, M. A.; Bauer, M.; Matukas, J.; Lisauskas, A.; Roskos, H. G.; Stake, J.Antenna-integrated 0.6 THz FET direct detectors based on CVD graphene. Nano Letters2014, 14, 5834–5838.

(24) Generalov, A. A.; Andersson, M. A.; Yang, X.; Vorobiev, A.; Stake, J. A 400-GHz GrapheneFET Detector. IEEE Transactions on Terahertz Science and Technology 2017, 7, 614–616.

(25) Bandurin, D. A.; Gayduchenko, I.; Cao, Y.; Moskotin, M.; Principi, A.; Grigorieva, I. V.;Goltsman, G.; Fedorov, G.; Svintsov, D. Dual origin of room temperature sub-terahertz pho-toresponse in graphene field effect transistors. Applied Physics Letters 2018, 112, 141101.

(26) Auton, G.; But, D. B.; Zhang, J.; Hill, E.; Coquillat, D.; Consejo, C.; Nouvel, P.; Knap, W.;Varani, L.; Teppe, F.; Torres, J.; Song, A. Terahertz Detection and Imaging Using GrapheneBallistic Rectifiers. Nano Letters 2017, 17, 7015–7020.

(27) Skoblin, G.; Sun, J.; Yurgens, A. Graphene bolometer with thermoelectric readout and capac-itive coupling to an antenna. Applied Physics Letters 2018, 112, 063501.

(28) Mics, Z.; Tielrooij, K.-J.; Parvez, K.; Jensen, S.; Ivanov, I.; Feng, X.; Mullen, K.; Bonn, M.;Turchinovich, D. Thermodynamic picture of ultrafast charge transport in graphene. NatureCommunications 2015, 6, 7655.

(29) Song, J. C. W.; Rudner, M. S.; Marcus, C. M.; Levitov, L. S. Hot carrier transport andphotocurrent response in graphene. Nano Letters 2011, 11, 4688–4692.

(30) Lemme, M. C.; Koppens, F. H.; Falk, A. L.; Rudner, M. S.; Park, H.; Levitov, L. S.; Mar-cus, C. M. Gate-activated photoresponse in a graphene p-n junction. Nano Letters 2011, 11,4134–4137.

(31) Gabor, N. M.; Song, J. C. W.; Ma, Q.; Nair, N. L.; Taychatanapat, T.; Watanabe, K.;Taniguchi, T.; Levitov, L. S.; Jarillo-Herrero, P. Hot Carrier-Assisted Intrinsic Photoresponsein Graphene. Science 2011, 334, 648–652.

(32) Cai, X.; Sushkov, A. B.; Suess, R. J.; Jadidi, M. M.; Jenkins, G. S.; Nyakiti, L. O.; Myers-Ward, R. L.; Li, S.; Yan, J.; Gaskill, D. K.; Murphy, T. E.; Drew, H. D.; Fuhrer, M. S. Sensitiveroom-temperature terahertz detection via the photothermoelectric effect in graphene. NatureNanotechnology 2014, 9, 814–819.

24

Page 25: Fast and sensitive terahertz detection using an antenna

(33) Guo, W.; Wang, L.; Chen, X.; Liu, C.; Tang, W.; Guo, C.; Wang, J.; Lu, W. Graphene-basedbroadband terahertz detector integrated with a square-spiral antenna. Optics Letters 2018,43, 1647.

(34) Goossens, S.; Navickaite, G.; Monasterio, C.; Gupta, S.; Piqueras, J. J.; Perez, R.; Burwell, G.;Nikitskiy, I.; Lasanta, T.; Galan, T.; et al., Broadband image sensor array based on graphene-CMOS integration. Nature Photonics 2017, 11, 366–371.

(35) Tielrooij, K. J.; Piatkowski, L.; Massicotte, M.; Woessner, A.; Ma, Q.; Lee, Y.; Myhro, K. S.;Lau, C. N.; Jarillo-Herrero, P.; van Hulst, N. F.; Koppens, F. H. L. Generation of photovoltagein graphene on a femtosecond timescale through efficient carrier heating. Nature Nanotechnol-ogy 2015, 10, 437–443.

(36) Zuev, Y.; Chang, W.; Kim, P. Thermoelectric and Magnetothermoelectric Transport Mea-surements of Graphene. Phys. Rev. Lett. 2009, 102, 96807.

(37) Tielrooij, K.-J.; Hesp, N. C. H.; Principi, A.; Lundeberg, M. B.; Pogna, E. A. A.; Banszerus, L.;Mics, Z.; Massicotte, M.; Schmidt, P.; Davydovskaya, D.; et al., Out-of-plane heat transferin van der Waals stacks through electronhyperbolic phonon coupling. Nature Nanotechnology2018, 13, 41–46.

(38) Bistritzer, R.; MacDonald, A. H. Electronic cooling in graphene. Physical Review Letters 2009,102, 13–16.

(39) Wang, L.; Meric, I.; Huang, P. Y.; Gao, Q.; Gao, Y.; Tran, H.; Taniguchi, T.; Watanabe, K.;Campos, L. M.; Muller, D. A.; Guo, J.; Kim, P.; Hone, J.; Shepard, K. L.; Dean, C. R.One-dimensional electrical contact to a two-dimensional material. Science 2013, 342, 614–7.

(40) Pizzocchero, F.; Gammelgaard, L.; Jessen, B. S.; Caridad, J. M.; Wang, L.; Hone, J.;Bøggild, P.; Booth, T. J. The hot pick-up technique for batch assembly of van der Waalsheterostructures. Nature Communications 2016, 7, 11894.

(41) Hwang, E. H.; Rossi, E.; Das Sarma, S. Theory of thermopower in two-dimensional graphene.Physical Review B - Condensed Matter and Materials Physics 2009, 80, 1–5.

(42) Mak, K. F.; Ju, L.; Wang, F.; Heinz, T. F. Optical spectroscopy of graphene: From the farinfrared to the ultraviolet. Solid State Communications 2012, 152, 1341–1349.

(43) Dawlaty, J. M.; Shivaraman, S.; Strait, J.; George, P.; Chandrashekhar, M.; Rana, F.;Spencer, M. G.; Veksler, D.; Chen, Y. Measurement of the optical absorption spectra ofepitaxial graphene from terahertz to visible. Applied Physics Letters 2008, 93, 131905.

(44) Lundeberg, M. B.; Gao, Y.; Woessner, A.; Tan, C.; Alonso-Gonzalez, P.; Watanabe, K.;Taniguchi, T.; Hone, J.; Hillenbrand, R.; Koppens, F. H. L. Thermoelectric detection andimaging of propagating graphene plasmons. Nature Materials 2017, 16, 204–207.

(45) Landau, L. D.; Bell, J.; Kearsley, M.; Pitaevskiii, L.; Lifshitz, E.; Sykes, J. Electrodynamicsof continuous media. Elsevier 1984, 8 .

(46) Cai, W.; Moore, A. L.; Zhu, Y.; Li, X.; Chen, S.; Shi, L.; Ruoff, R. S. Thermal transportin suspended and supported monolayer graphene grown by chemical vapor deposition. NanoLetters 2010, 10, 1645–1651.

25

Page 26: Fast and sensitive terahertz detection using an antenna

(47) Koh, Y. K.; Bae, M. H.; Cahill, D. G.; Pop, E. Heat conduction across monolayer and few-layergraphenes. Nano Letters 2010, 10, 4363–4368.

(48) Tan, Y. W.; Kim, P. Measurement of Scattering Rate and Minimum Conductivity in Graphene.Phys. Rev. Lett. 2007, 99, 246803.

(49) Lee, J. E.; Ahn, G.; Shim, J.; Lee, Y. S.; Ryu, S. Optical separation of mechanical strain fromcharge doping in graphene. Nature Communications 2012, 3, 1024–1028.

(50) Lundeberg, M. B.; Koppens, F. H. L. Thermodynamic reciprocity in scanning photocurrentmaps. 2018, In preparation.

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