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COMMUNICATION
Phototransistors
www.advopticalmat.de
High Performances for Solution-Pocessed 0D–0D
Heterojunction Phototransistors
Yu Yu, Yating Zhang,* Xiaoxian Song, Haiting Zhang, Mingxuan Cao, Yongli Che,
Haitao Dai, Junnbo Yang, Heng Zhang, and Jianquan Yao
narrow band emission, low-cost, and the
facile synthesis process.[1–5] As one of the
all-inorganic PQDs, CsPbBr3 with high
carrier mobility up to ≈4500 cm2 V−1 s−1[6]
offered a large bandgap of 2.29 eV. The
proper bandgap, large surface-to-volume
ratio, and high mobility enabled it as a
promising material for optoelectronic
application fields.[7] Recently, phototransistors based on CsPbBr3 PQDs have been
investigated, while most of them show
low responsivity up to ≈0.64 A W−1 and
the response time in the order of microseconds.[8] Hu and co-workers[9] demonstrated phototransistor based on CsPbBr3
PQDs, exhibiting that the detection spectrum ranges from 380 to 600 nm and the
decay time was determined to be ≈15 ms.
Ramasamy et al.[10] reported photodetectors fabricated from CsPbI3 PQDs exhibiting that the good ON/OFF photocurrent
ration of 105 and rise time and decay times
of 24 and 29 ms, respectively. The reported
responsivity of CsPbBr3 PQDs devices
were limited by their trade-off dependence. In addition, it also
suffered from weak light absorption and narrow response
range. Therefore, hunting a moderated sensitized material to
combine with CsPbBr3 PQDs held great potential to improve
the detection performances.
Low cost and solution processed colloidal quantum dots
(CQDs) have enabled photodetectors[11] that benefit from
infrared sensitivity,[12] high light absorption,[13] wavelength
tenability.[14] Exhibiting tunable bandgap from 0.5 to 1.7 eV[15]
matching PQDs’ energy level and high air stability with organic
ligands, PbS colloidal quantum dots[16–24] have a significant
absorption capacity for NIR and short-wavelength light, which
PQDs can’t be access to. The reported photoconductive detectors based on hybrid PbS QDs/graphene have achieved a
responsivity up to 107 A W−1 attributed to the photogating
effect through capacitive coupling.[25] While most of graphenebased devices suffered from the high dark current, low on–off
ratio (<2) and slow response speed due to the semimetal channels.[26–29] In order to suppress the response times by decorating CQDs with 2D WS2 channel, we introduced PbS QDs/
WS2 hybrid phototransistor with improved electrical bandwidth
and response time.[30] As our knowledge, broadband phototransistors based on CsPbBr3–PbS CQDs heterostructure have
never been reported.
All-inorganic cesium lead halide perovskite nanocrystals have emerged as
attractive optoelectronic nanomaterials due to their stabilities and highly
efficient photoluminescence. High-sensitivity photodetection covering a large
spectral range from ultraviolet to near-infrared is dominated by phototransistors. To overcome existing limitations in sensitivity and cost of state-of-the-art
systems, new-style device structures and composite material systems are
needed with low-cost fabrication and high performance. Here, field-effect
phototransistors (FEpTs) based on CsPbBr3–PbS colloidal quantum dot
heterostructure dominate to obtain a wide response spectral range and high
performance. The large spectral detection spectrum is from 400 to 1500 nm
similar to PbS quantum dots’ response. It is worth mentioning that the device
shows responsivity up to 4.5 × 105 A W−1, which is three orders of magnitude
higher than the counterpart of individual material-based devices. Furthermore, other high performance of hybrid CsPbBr3–PbS FEpTs including a short
photoresponse time (less than 10 ms) is ascribed to the assistance of heterojunction on the transfer of photoexcitons. The solution-based fabrication
process and excellent device performance strongly underscore CsPbBr3–PbS
quantum dot as a promising material for future photoelectronic applications.
Colloidal all-inorganic cesium lead halide (CsPbX3, X = Cl, Br,
and I) perovskite quantum dots (PQDs) have attracted a great
scientific attention in photovoltaic devices due to their excellent properties, such as the large bandgap, tunability, efficient
Dr. Y. Yu, Dr. Y. Zhang, Dr. X. Song, Dr. H. Zhang, Dr. M. Cao, Dr. Y. Che,
Dr. H. Zhang, Prof. J. Yao
Institute of Laser & Opto-Electronics
College of Precision Instruments and Opto-electronics Engineering
Tianjin University
Tianjin 300072, China
E-mail: yating@tju.edu.cn
Prof. H. Dai
Tianjin Key Laboratory of Low Dimensional Materials Physics
and Preparing Technology
School of Science
Tianjin University
Tianjin 300072, China
Prof. J. Yang
Center of Material Science
National University of Defense Technology
Changsha 410073, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adom.201700565.
DOI: 10.1002/adom.201700565
Adv. Optical Mater. 2017, 1700565
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© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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Figure 1. a) The schematic diagram of CsPbBr3–PbS hybrid phototransistor architecture. b) X-ray diffraction spectrum of the CsPbBr3–PbS film, (inset:
the SEM image top-view of perovskite on silicon substrate). c) Optical absorption spectrum of hybrid including perovskite and PbS quantum dots on
glass substrate. d) Logarithmic plot of the transfer characteristics of typical CsPbBr3 phototransistors, before (in darkness) and after PbS quantum
dots decoration (in darkness and under illumination of 845 mW cm−2) with VDS = 0.24 V applied bias voltage.
Hence, we fabricated hybrid phototransistors based on the
high transport mobility CsPbBr3 PQDs and PbS QDs for high
performance and broadband detection. The hybrid phototransistor demonstrated responsivity up to 4.5 × 105 A W−1 and a
specific detectivity of 7 × 1013 Jones, which were much higher
than those of control devices. The enhancement mechanism
was attributed to the coupling effect introduced by hybrid
device structure and their type-II energy band alignment. The
phototransistor exhibits fast response times (a rise time of
6.5 ms and a decay time of 7.5 ms), and excellent stability and
reproducibility. The hybrid device structure, superior detection
performance, and versatile working state promise great potential for future optoelectronic devices.
The schematic diagram of heterojunction phototransistor coupled by CsPbBr3 PQDs and PbS QDS is depicted
in Figure 1a. The source and drain electrodes of Cr/Au were
deposited through a thermal evaporation method assisted by
a shadow mask, where the channel length (L) and channel
width (W) were defined as 0.1 and 2.5 mm, respectively. Then
the colloidal CsPbBr3 perovskite QDs made by room temperature synthesis (see Supporting Information for details) were
spin-coated on the device with the rotating speed of 2000 rpm
min. Finally, the as-synthesized colloidal PbS QDs (the preparation and deposition are referred to Supporting Information
for detail) were uniformly deposited by spin coating method
on CsPbBr3 perovskite QDs and the coated QDs ligands were
exchanged by ethanedithiol. For the bottom-gate configuration,
a highly doped n-type silicon wafer covered with a 300 nm thick
SiO2 layer (capacitance Cox of 11.5 nF cm−2) was used as gate
Adv. Optical Mater. 2017, 1700565
electrode. Notably, the thickness of photosensitive layer is a key
parameter for phototransistors. It will have a significant impact
on abilities either absorbing light or gate electrode modulation.
Specially, if the photosensitive layer is too thin (4–7 nm for our
devices in our experiments) to absorb sufficient light to convert photoexcitons. In addition, pinholes in this PQDs film will
cause inhomogeneous conduction in the channel. While if the
film is too thick (>20 nm for our devices), and the bottom gate
will not effectively modulate the channel. Therefore, in this
paper, the optimized thickness of the CsPbBr3 PQDs film as the
channel material in the phototransistor was fixed at ≈15 nm.
(see Supporting Information for details). The transmission
electron microscopy image in Figure 1b depicts cubic shape of
CsPbBr3 PQDs.[1,4] As shown in the inset of Figure 1b, a lattice spacing of 0.499 nm, corresponding to the (200) plane, was
clearly observed, which revealed that the CsPbBr3 PQDs were
highly crystalline. The absorption region ranges from visible to
near-infrared wavelength, depicted in Figure 1c, indicating that
this device can be used for broadband spectrum detection. The
hybrid shows two absorption peaks – “510” and “1310” nm –
between 300 and 1500 nm. For the measurement details, the
source (with ground connection) and drain electrodes were connected with Keithley 2400, and the channel current flowing into
the drain electrode (IDS), which was also measured by Keithley
2400, and the gate voltage (VGS) was applied by HP6030A. The
photoelectrical measurements were also performed based on
this system under illumination of 405, 532, and 808 nm lasers.
The transfer characteristics of typical pritime CsPbBr3 perov­
skite QDs phototransistors, before (in darkness: red line) and
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after PbS quantum dots decoration (in darkness: black line and
under illumination of 845 mW cm−2: green line) with applied
bias voltage VDS = 0.24 V are depicted in Figure 1d, respectively. Each device exhibits typically ambipolar characteristics,
and a “V” shape of the transfer curves is particularly presented,
manifesting either electrons or holes transport in the n-type
or p-type channels of the device, respectively. Particularly, for
the CsPbBr3–PbS phototransistor, the mechanism can be interpreted that after the two materials contact with each other,
owing to the difference of electron potentials, the electrons are
injected into CsPbBr3. Therefore, as the conventional theory
of heterojunction contacts, a built-in-electric field is formed at
the interface, and the direction points from PbS to CsPbBr3.
Upon illumination, electrodes separated from photoexcitons
generated in heterojunction should flow into PbS. However,
this is opposite to our experimental results. Different from the
traditional energy theory, the CsPbBr3–PbS heterostructures
are atomic layers, and the depletion region of the heterojunction is so thin that the charge concentration and polarity at the
interface of CsPbBr3–PbS should be liable to be affected by the
charge imparities on the surfaces of CsPbBr3 PQDs and PbS
QDs or the applied electrostatic field.[31] A cascade-like alignment of the conduction band would thereby improve the electron transfer toward the channel−QD junction and increase
the charge collection efficiency, allowing thicker QD films
with higher absorption.[32] The applied electric field and the
external electric field that is from an effective electric field at
the CsPbBr3–PbS interface. The effective electric field determines the following direction and an amount of the electrodes
separated from photoexcitons tend to reside in the PQDs layer.
Therefore, the shift toward negative VGS (shown in Figure 1d)
can be ascribed to the efficient photoexcitons separation and
holes transfer at the interface.[33] Comparing with the condition
with no irradiation, the values of |IDS| become larger. It can be
understood that the photoinduced carriers can be generated
under the condition of light irradiation. Therefore the enhancements of IDS are ascribed to the increase of the electron and
hole concentrations. Meanwhile, the field-effect mobility and
gate voltage can be extracted with the equation of
µ=
L
∂I DS
VDSC oxW ∂VGS (1)
where W, L, and Cox are the channel width, channel length, and
the gate capacitance per area, respectively. Therefore, the carrier mobilities[34] can be calculated as 4083 cm2 V−1 s−1, which
is larger than prior studies in pristine PbS QDs phototransistor (0.01 cm2 V−1 s−1),[35] respectively. Figure S5 in the Supporting Information shows the I–V curves of the PbS–CsPbBr3
QDs heterojunction phototransistor at different gate voltages
(±0.5, ±1, ±1.5, ±2, ±2.5, ±3 V). If VGS > 0, the positive gate
voltage (VGS) can induce large amounts of electrons in the
interfaces between the CsPbBr3 QDs and SiO2 substrate, and
a conducting channel is created which allows the current to
flow between the source and drain. The feild effect transistors
(FETs) operate like a resistor and work at linear region, thus
the source-drain current (IDS) can linearly depend of sourcedrain voltage (VDS) as shown Figure S5 in the Supporting Information under the condition of relatively small drain-source
voltage. If VGS and VDS are both negative, the device operates in
the hole-enhancement mode, while both are positive, the device
operates in the electron-enhancement mode. Specially, at low
|VGS| (Off-state), IDS increases rapidly with the increase of VDS,
indicating that a Schottky barrier forms in the device. However,
at high |VGS| (ON-state), similar to traditional FETs with linearto-saturation current-voltage characteristics, the device exhibits
unipolar transport properties.
The dark currents and photocurrents of each phototransistor
across a wide range of wavelengths with the same irradiation
are measured. Photoresponsivity (R) is calculated by
∆I DS I illu − I dark
=
(2)
P
Ee × S where Iillu and Idark represent the drain current under illumination and in the darkness. P, Ee, and S are power density,
irradiance, and the effective channel area, respectively. The
photoresponsivity of CsPbBr3–PbS hybrid phototransistor and
pristine PbS phototransistor as the function of wavelength are
respectively shown in Figure 2a. As to the broad absorption
of PbS QDs, it was expected the CsPbBr3–PbS hybrid device
could inherit the wide spectra detection. Ranging from 400
to 1500 nm, the phototransistor exhibits a broadband photoresponse and is suitable for visible light to near-infrared
light photodetection, which is determined by the absorption
curve of hybrid film in Figure 1c. The responsivity spectrum
R=
Figure 2. a) The photoresponsivity (R) of the devices at different wavelengths from 400 to 1500 nm at a bias of 2 V and zero applied gate bias.
b) Photoresponsivity (R) of the hybrid device at a wavelength of 808 nm as a function of Ee under the condition of VDS = 2 V, VGS = 3 V. Inset: photocurrent for different illumination intensities.
Adv. Optical Mater. 2017, 1700565
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Figure 3. Photoresponse characteristics of perovskite phototransistor under irradiation with red light (λ = 808 nm). a) Current response of the device
with a red light irradiance of 845 mW cm−2. b) Temporal photocurrent responses highlighting a rise time of 6.5 ms and a decay time of 7.5 ms.
photocurrents. However, for higher light irradiances, some
for CsPbBr3 phototransistor ranges from 400 to 800 nm, and
photoexcitons remained in the trap states[37] of perovskite, thus
a peak response at about 510 nm. Particularly, the maximum
−1
photoresponsivity (R) is only calculated 1.0 A W at 400 nm.
cannot be converted to the photocurrent, leading to the saturation of photocurrent shown in the inset of Figure 2b. As for
While for the hybrid CsPbBr3–PbS phototransistor the detection spectrum ranges from 400 to 1500 nm, and the maximum
R, the R decreases if Ee increases in a reciprocal function of
n
photoresponsivity can be reached to 4.5 × 105 A W−1. Other key
E
R = a /1 +  e  , where a and b are constants and n is a logistic
parameters characterizing photodetector’s performance, such
 b
as the detectivity (D*), the noise equivalent power, the gain
fitting parameter. It indicates a linear relation between R and Ee
[36]
*
1/2
1/2
1/2
*
(G) can be given as D = RA /(2eI DS ) , NEP = A /D ,
is shown in the double logarithmic axis coordinate of Figure 2b.
hν
According to the theory[38–40]
and G =
R , respectively, where R is the responsivity, A is the
e
area of the detector, e is the charge of an electron, and IDS is
1
 e T0 
R=
the dark current. The D*, NEP, and G of the device are 1.26
n
(3)
 hν Tr 
P
13
−17
−1
6

× 10 Jones, 3.97 × 10 W Hz , and 1.4 × 10 , respectively.
1+  
 P0 
The responsivity of each device exhibits a decreasing trend,
and it is reasonable since the photocurrent generation needs
where e is the electron charge, hν is the energy of single
to match the basic condition, that is, the incident photo energy
photon, T0 is the carrier lifetime, Tr is the carrier transfer time,
must be larger than the energy gap. Only these incident photos
P0 is the excitation intensity where the surface states are fully
with enough photon energy can excite electrons from the valfilled, and n is a phenomenological fitting parameter. The red
ance band maximum (VBM) to the conduction band minimum
solid line in the inset of Figure 2b is the best fit to the data
(CBM), generating the photocurrent when the drain voltage is
obtained by Equation (3) from which P0 = 0.01 W, and n = 1
applied. Therefore, more electrons and photoexcitons can be
have been deduced.
excited with larger incident photo energy lights in the short
As another key parameter for photodetector, photoresponse
wavelength and contribute more to photocurrent. It indicates
speed determines the capability of a photodetector to follow a
that electrons have to overcome the Schottky barrier during
fast-switching optical signal. In order to highlight the photoretransporting. Under the illumination of larger energy light in
sponse of the device during IR spectrum, initially we exploit
the shorter wavelength, the built in potential of the Schottky
pump laser with an excitation wavelength of 808 nm, which
barrier decreases, resulting in a large increase in the free caris below the absorption edge of PbS (shown in Figure 1c).
rier density, leading to the easier carriers transport and tunFigure 3a shows drain current response of the device with light
neling, thus, to greatly enhanced photocurrents.
irradiance of 845 mW cm−2, exhibiting stable and reproducible
Figure 2b exhibits the photocurrent and responsivity (R)
of the device with the relation of irradiance
(Ee), in which the photocurrent increases lin- Table 1. Comparison in device performance of CsPbBr /PbS hybrid FEpTs with its single
3
early with Ee at low light irradiance, while it counterparts.
deviates below this linearity at higher light
irradiation. It is concluded that with larger Device
Response times
Charge mobility Spectral coverage Maximum responsivity
irradiance more photoexcitons and elec[nm]
[A W−1]
[cm2 V−1 s−1]
trons can be excited, leading to the decrease CsPbBr3
4500
400–800
1
Almost none response to
of built in potential of the Schottky barrier,
808 nm
which have a higher probability to overpass PbS
20 s/28 s
0.01
400–1500
2 × 102
the Schottky barrier, and then flow to the
4083
400–1500
6.5 ms/7.5 ms
4.5 × 105
external circuit to generate linearly enhanced CsPbBr3/PbS
Adv. Optical Mater. 2017, 1700565
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Figure 4. Electronic band structure and working principle of the CsPbBr3–PbS bilayer phototransistor under the illumination of a) hν > 2.3 eV and
b) 0.9 eV < hν < 2.3 eV.
photoresponse. The drain current quickly increases as soon
as the light switch is turned on and then decreases when the
light switch is turned off. It indicates that the increased charge
intensity will lower the effective barrier height upon illumination, which allows easier charge tunneling and transportation
than that of device in darkness.
Figure 3b shows the temporal photocurrent response of
the device. The rise and decay times of the photocurrent are
≈6.5 and 7.5 ms, respectively. Recently, using pristine perov­
skite, Song et al.[8] reported switching times of phototransistors
are ≈19 and 25 µs. It is reasonable that the speed is probably
limited by the lower charger mobility of the PbS QDs layer
(carrier mobilities ≈0.03 (hole) cm2 V−1 s−1 and ≈0.01 (electron)
cm2 V−1 s−1) and some photo carriers remain trapped in the
perovskite channel, resulting in increased carrier lifetime. To
demonstrate the breakthrough improvement achieved by this
hybrid, we fabricated different devices, with similar method
and CsPbBr3 perovskite as the only active layer (Figure S3, Supporting Information) or hybrids isolated CsPbBr3 perovskite
film (Figure S4, Supporting Information). To compare with
characteristics based on CsPbBr3 perovskite and PbS QDs
alone, several key parameters[41] are listed in Table 1.
The sensing mechanism of CsPbBr3/PbS hybrid FEpTs can
be schematically described in Figure 4. If the incident photon
energy is greater than bandgap of CsPbBr3 PQDs, which is
2.25 eV[42] (shown in Figure S1a in the Supporting Information),
that is, 551 nm in wavelength, electrons and hole (photo excitons) are generated. While for PbS QDs, the bandgap is 0.9 eV,
that is, 1.37 µm in wavelength. Particularly, only these incident
photons with larger energy (hν > 2.25 eV, that is, wavelength <
551 nm) can excite electrons from the VBM to the CBM in the
CsPbBr3 PQDs, generating the photocurrent if the drain voltage
is applied. Given the CBM of PbS QDs is lower than that of
CsPbBr3 PQDs, photogenerated electrons can roll down to the
CBM of PbS. However, the VBM of PbS is larger than that of
perovskite, therefore, the photogenerated holes in CsPbBr3
PQDs can be energetically transferred to PbS QDs. Due to the
larger hole mobility in perovskite, the holes drift faster in perov­
skite than that in PbS, and can be rapidly collected by the electrodes. And the charges transfer at the PbS/perovskite interface, leading to the formation of depletion layer. And the depletion layer assists in the charge separation. Meanwhile, three
Adv. Optical Mater. 2017, 1700565
occasions need to discuss due to different energy gaps (Eg)
of perovskite and PbS. If hν is larger than 2.25 eV, shown in
Figure 4a, electron–hole pairs are generated in perovskite and
PbS QDs films, and the electrons (holes) are transferred to PbS
film, which lowers (raises) the Fermi level of PbS and reduces
the Schottky barriers, resulting in the high photocurrent.
While hν is larger than 0.9 eV smaller than 2.25 eV, shown
in Figure 4b, electron–hole pairs can be excited only in PbS
film. Therefore, the photocurrents become small. And if hν is
smaller than 0.9 eV, none electron–hole pairs are generated so
the photocurrent approximately equals dark current.
In summary, broadband phototransistors based on CsPbBr3
perovskite-PbS colloidal quantum dots heterostructures were
fabricated through a low-cost, solution-processed strategy. The
phototransistor exhibits bipolar behaviors and a wide spectral
response—from 400 to 1500 nm. Particularly, the phototransistor is photoresponsive to the UV (405 nm), VIS (532 nm),
and NIR (808 nm) irradiations, and presents stability and reproducibility in the progress of ON–OFF cycles. Carrier mobility
of CsPbBr3–PbS heterojunction photodetector is measured
as 4083 cm2 V−1 s−1. It is worth mentioning that the fast rise
and decay times of the photocurrent are ≈ 6.5 ms and 7.5 ms,
respectively. Therefore, these results indicate that solutionbased process perovskite-PbS colloidal quantum dots heterostructures have great potential applications for ultrabroadband
photodetection, especially in the IR region.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was supported by the National Natural Science Foundation of
China (Grant Nos. 61675147 and 61605141).
Conflict of Interest
The authors declare no conflict of interest.
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Keywords
broadband phototransistors, heterojunctions, inorganic perovskite
quantum dots
Received: June 16, 2017
Revised: September 2, 2017
Published online:
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