highly sensitive photodetectors based on hybrid 2d-0d sns2 … · 2017. 5. 18. · highly sensitive...

Highly sensitive photodetectors based on hybrid 2D-0D SnS2-copper indium sulfidequantum dotsYun Huang, Xueying Zhan, Kai Xu, Lei Yin, Zhongzhou Cheng, Chao Jiang, Zhenxing Wang, and Jun He Citation: Applied Physics Letters 108, 013101 (2016); doi: 10.1063/1.4939442 View online: http://dx.doi.org/10.1063/1.4939442 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/108/1?ver=pdfcov Published by the AIP Publishing Articles you may be interested in High-performing visible-blind photodetectors based on SnO2/CuO nanoheterojunctions Appl. Phys. Lett. 107, 241108 (2015); 10.1063/1.4938129 Suppression of dark current through barrier engineer for solution-processed colloidal quantum-dots infraredphotodetectors Appl. Phys. Lett. 107, 091115 (2015); 10.1063/1.4930158 Bulk- and layer-heterojunction phototransistors based on poly [2-methoxy-5-(2′-ethylhexyloxy-p-phenylenevinylene)] and PbS quantum dot hybrids Appl. Phys. Lett. 106, 253501 (2015); 10.1063/1.4922917 Ultraviolet emission from low resistance Cu2SnS3/SnO2 and CuInS2/Sn:In2O3 nanowires APL Mater. 2, 116107 (2014); 10.1063/1.4901295 Quantum dot nanocolumn photodetectors for light detection in the infrared Appl. Phys. Lett. 92, 261113 (2008); 10.1063/1.2949084

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Highly sensitive photodetectors based on hybrid 2D-0D SnS2-copper indiumsulfide quantum dots

Yun Huang,a) Xueying Zhan,a) Kai Xu, Lei Yin, Zhongzhou Cheng, Chao Jiang,Zhenxing Wang,b) and Jun Heb)

CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscienceand Technology, Beijing 100190, China

(Received 28 September 2015; accepted 19 December 2015; published online 4 January 2016)

Both high speed and efficiency of photoelectric conversion are essential for photodetectors. As an

emerging layered metal dichalcogenide (LMD), tin disulfide owns intrinsic faster photodetection

ability than most other LMDs but poor light absorption and low photoelectric conversion efficiency.

We develop an efficient method to enhance its performance by constructing a SnS2-copper indium

sulfide hybrid structure. As a result, the responsivity reaches 630 A/W, six times stronger than pristine

SnS2 and much higher than most other LMDs photodetectors. Additionally, the photocurrents are

enhanced by more than 1 order of magnitude. Our work may open up a pathway to improve the

performance of photodetectors based on LMDs. VC 2016 AIP Publishing LLC.[http://dx.doi.org/10.1063/1.4939442]

Earth-abundant layered metal dichalcogenides (LMDs)

with general formula MX2 (M¼Mo, W, Sn, Ti, Zr, Hf, Nb,Ta, and X¼S, Se) have attracted a great deal of attentionover the past decade.1–3 The nature of suitable band-gaps and

monolayer-stability enable them ideal candidates for applica-

tion in photodetection, which require high performance in

terms of speed and efficiency of photoelectric conversion.

Motivated by those targets, a great number of photodetectors

based on LMDs, such as MoS2 and WSe2, have been fabri-

cated.4–7 However, a few of them can meet both. As an impor-

tant member of LMDs, tin disulfide (SnS2) has attracted

increasing attention recently. Field effect transistors (FETs)

based on exfoliated SnS2 Nanosheets (NSs) show high on/off

ratio� 106 and mobility up to 230 cm2 V�1 s�1 at room tem-perature.8–10 Monolayer to few-layer SnS2 NSs have been

synthesized by chemical vapor deposition (CVD) on carbon

fiber, mica, and silicon substrates.11–13 SnS2 NSs especially

can behave similar to ultrafast photodetectors with the rising

time� 5 ls,14 which is at least an order of magnitude fasterthan those based on MoS2, WS2, GaTe, and many other lay-

ered materials,6,15,16 indicating its great superiority as ultra-

sensitive photodetectors. However, its responsivity is limited

to 8.8 mA/W. Recently, we synthesized thin SnS2 NSs on car-

bon fibers though a CVD method and verified its potential in

fast and sensitive phototransistors.11 But the indirect bandgap

nature of SnS2 may hinder the photoelectric conversion effi-

ciency from meeting a higher standard. Thus, it is of great

value to explore a strategy that improves the light absorption

of SnS2 photodetectors.

On the other hand, 2D-0D hybrid architectures have

recently received considerable attention for their high per-

formance as photodetectors.17–20 This structure benefits from

strong light absorption, facile bandgap tunability, large

scale manufacturability of quantum dots (QDs),21,22 and the

facilitative separation of photoexcited charges induced by

type II heterojunction formed between the QDs and the lay-

ered materials. Besides, with the single crystal layered mate-

rial as a channel, this structure also avoids the boundary

issues in QDs photodetectors. As a result, the responsivity of

the hybrid graphene-PbS phototransistors could be 107 A/W

with fast response time�10 ms.17 A hybrid MoS2-PbS QDsphotodetector could show high responsivity of 105–106 A/W

as well as fast response time�0.35 s.18 Accordingly, wedesigned a hybrid device combined p-type copper indium sul-

fide (CuInS2, CIS) QDs with the CVD-grown SnS2 NSs. The

schematic of the hybrid device is shown in Fig. 1(a). The CIS

QDs have demonstrated fruitful application in solar cell for its

high light absorption and chemical stability.23–26 Besides,

with its proper energy band structure, CIS-decorated SnS2could form a typical type-II band alignments,27 as shown in

Fig. 1(b), which helps to improve photoresponse of SnS2.

Herein, we report a photodetector based on SnS2-CIS

QDs hybrid architecture. Due to the type II heterojunction

formed between SnS2 and CIS QDs, the device exhibits

enhanced light absorption ability, fast photoresponse, sensitive

and gate-tunable photodetection. It is also notable that the

responsivity reaches as high as 630 A/W at P¼ 2.83 mW/cm2,which is comparable with that of graphene-PbS hybrid photo-

detection at the same power of illumination. Thus, our study

may provide a method to improve the performance of photo-

detectors and expand the building blocks for high performance

optoelectronic devices.

The SnS2 NSs were synthesized by a CVD method as

reported in our previous work.11 The CIS QDs were synthe-

sized through a solvothermal recipe. In a typical process,

0.33 g CuCl2, 0.81 g InCl3, and 1.04 g SC(NH2)2 were added

to 3 ml alcohol and 40 ml deionized water in a 50 ml Teflon

autoclave. Then the reactor was maintained at 240 �C for 3 h.After that, �10 nm CIS QDs were precipitated at the bottomof the reactor. To fabricate device, as-grown thin SnS2 NSs

were drop-casted onto p-doped silicon substrates with

300 nm thick thermal oxidation layer. A standard e-beam

a)Y. Huang and X. Zhan contributed equally to this work.b)Authors to whom correspondence should be addressed. Electronic addresses:

[email protected] and [email protected]

0003-6951/2016/108(1)/013101/5/$30.00 VC 2016 AIP Publishing LLC108, 013101-1

APPLIED PHYSICS LETTERS 108, 013101 (2016)


02:49:46

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lithography (EBL) process was carried to define the electri-

cal metal electrodes. Cr/Au (5 nm/80 nm) metal electrodes

were deposited by thermal evaporation. After the measure-

ment of pristine SnS2 device, CIS QDs were spin-coated

onto its surface, using a method similar with Ref. 17. During

this procedure, 20 mg CIS QDs were dissolved in 5 ml tolu-

ene and centrifuged at 3000 rpm for 30 s. Then two drops

(each drop�0.05 ml) of the supernatant was dropped ontothe rotating substrates (2000 rpm) followed by 3 drops of 2

vol. % 1,2-ethanedithiol-ligands (EDT) in acetonitrile and

another 2 drops of acetonitrile and toluene. This sequence

was repeated for 3 times. Then, the substrate was dried at

30 �C for 10 min.Transmission electron microscope (TEM) and Raman

spectrum were used to characterize our synthesized SnS2 NSs

and CIS QDs. Fig. 1(c) exhibits the HRTEM of the SnS2 NSs

(top panel) and CIS QDs (bottom panel). The high crystallin-

ity of the SnS2 NSs could be concluded from the regular dif-

fraction fringes with the lattice spacing of 3.15 Å indexed to

the (100) plane.28 Meanwhile, the lattice constant�3.18 Å inFig. 1(c) (bottom panel) agrees well with the (112) plane of

CIS.25 Raman spectra of SnS2 NSs, CIS QDs, and the hybrid

structure are shown in Fig. 1(d), respectively. It is clear that

the Raman spectrum of the hybrid structure shows two peaks

assigning to that of SnS2 nanosheets (313.6 cm�1) and CIS

(303.2 cm�1).14,29 The UV-visible-IR absorption spectroscopy

of SnS2 and hybrid SnS2-CIS quantum dots in Fig. 1(e) veri-

fies that the light absorption range of hybrid SnS2-CIS is

enhanced and extended to part of the near infrared (NIR)

region after CIS QDs deposition.

To investigate the performance of SnS2-CIS hybrid pho-

todetector, photoresponse of the pristine and hybrid device

under 473 nm laser were conducted, respectively. Noting

that our previous work has demonstrated oxygen molecules

in ambient could grab electrons from the n-type channel

materials and thus seriously affect the properties of the de-

vice,11,20,30 all the measurements in our experiment were

carried in vacuum �10�5 Torr. The inset of Fig. 2(a) showsan atomic force microscope (AFM) image of the pristine

device, indicating the thickness of the channel SnS2NSs� 13.6 nm. The I-V curves of the same photodetectorbefore and after CIS QDs deposition in the dark and under

laser illumination are shown in Fig. 2(a). It is obvious that

the dark currents of hybrid device slightly increase while the

photocurrents dramatically augment by at least one order.

This increase could also be verified by the photoresponse of

the hybrid and pristine device under different power of inci-

dent illumination, as shown in Fig. 2(b). After decorating

with CIS QDs layer, the sensitivity of the SnS2 device

remained, embodying in the increasing photocurrents as the

power of incident illumination increases. Furthermore, as a

critical parameter for photodetector, the responsivity (Rk) ofthe device was improved. The Rk can be calculated as thefollowing formula:31

Rk ¼ Iph=PS; (1)

where Iph is the photocurrents and P and S are effective illu-mination intensity and area. As plotted in Fig. 2(c), the high-

est responsivity of the hybrid device reaches as high as

630 A/W at P¼ 2.83 mW/cm2, while that of the pristine de-vice is 167 A/W. The time-resolved photoresponse of the de-

vice (Fig. 2(d)) shows that after QDs deposition, the rising

and decay time could remain within 110 ms. Meanwhile, no

obviously slow decay tail was observed,32 indicating the

potential of the hybrid device for sensitive photodetectors.

Here, the enhanced photocurrents and responsivity origin

from the designed type II structure. Band bending induced

build-in field between the interface of CIS and SnS2 drives

the photogenerated electrons and holes to move in opposite

directions, reducing the recombination rate significantly. The

electrons transferred from CIS to SnS2 can increase the

charge density of the channel material, leading to higher

photocurrents. Meanwhile, the holes are trapped in the CIS

FIG. 1. Device schematics and charac-

teristics. (a) Schematic diagram of a

SnS2-CIS QDs hybrid device under

illumination. (b) Band-diagram of

the hybrid device under light illumina-

tion. (c) HRTEM of as-grown SnS2NSs (upper) and CIS QDs (lower). (d)

Raman spectra of the SnS2 NSs, CIS

QDs, and the hybrid device. (e) The

UV-visible-IR absorption spectroscopy

of SnS2 and hybrid SnS2-CIS quantum

dots.

013101-2 Huang et al. Appl. Phys. Lett. 108, 013101 (2016)


02:49:46

film, which further serve as an effect of photogating and lead

to the transfer threshold voltage shift. It could also explain

the background photocurrents change shown in Fig. 2(b).33

As shown in our previous work, SnS2 displays great

potential as phototransistors with sensitive light response and

gate tunable photoswitch ratio.11 We further verify that its

performance could be improved with hybrid architecture.

Transfer curves with or without light illumination were meas-

ured before and after QDs deposition. Considering possible

gate hysteresis, all the curves are acquired as the gate voltage

was applied from negative to positive values. The hybrid de-

vice shows increased currents both in the dark and under illu-

mination, as presented in Fig. 3(a). Besides, the threshold

voltage shifts from 19.9 V to 8.81 V after QDs deposition,

indicating an obvious electron doping effect. It is notable that

our hybrid device exhibits positive photoconductivity in the

whole range of gate sweeping, significantly different with

Ref. 18, in which the MoS2-PbS QDs photodetectors exhibit

positive photoconductivity only at strong negative Vgs.18 As

plotted in Fig. 3(b), the hybrid device remains sensitive photo-

response compared with the pristine device, showing increas-

ing currents as the power of illumination increases. Even

though the pristine device shows a relatively higher responsiv-

ity than many other LMDs,5,34,35 the responsivity of the

hybrid device is still improved by several to ten times. Figs.

3(c) and 3(d), respectively, depict the responsivity of device

before and after CIS QDs deposition as the power of illumina-

tion increases. We draw these two figures in the same

range (101 mA/W–106 mA/W) to facilitate a comparison. The

highest responsivity measured of hybrid phototransistors is

500 A/W at P¼ 5.94 mW/cm2, Vgs¼ 50 V. Though severalother hybrid devices have shown a responsivity as high as

107 A/W, the results were measured at a very low intensity of

illumination.17–20 Our results are comparable with that of

those hybrid phototransistors at the same intensity of illumina-

tion. Besides, it is obvious that the measured responsivity

displays a tendency of increasing as the intensity of illumina-

tion decreases. At higher illumination intensity, more photo-

generated charges are separated, which induce an increasing

reverse electric field. As a result, the build-in field is lowered,

leading to accelerating charges recombination at the interface

and dropping responsivity. Thus, it is safe to predict that our

hybrid device would show even higher responsivity at an illu-

mination of lower intensity.

Another interesting phenomenon is that the transfer

curves shift as the intensity of illumination increases, as indi-

cated in Fig. 3(b). For one reason, photogenerated electrons

transfer from the CIS layer to SnS2, which results in more

electrons in the channel. For another reason, photogenerated

holes remained in the CIS QDs layer, leading to a photogat-

ing effect, which further changes the conductance of the

channel material through capacitive coupling.17,36 As a

result, the threshold voltage of the hybrid device shifts to

negative gate voltages. To clearly show these collaborative

effects, we plot the threshold voltage shift as a function of

light illumination in Fig. 4(a). Interestingly, the curve can be

fitted very well with the following equation, which has been

used for phototransistors before:19,37

DVth ¼ aPb; (2)

where DVth is the shift of threshold voltage, P is the intensityof light illumination, and a and b are the constant. Besides, itis well known that the channel current could be expressed as38

Ids ¼W

LlCox VG � VT �

VD2

� �VD; VD � VG � VTð Þ;

(3)

where Cox is the capacitance of the gate dielectric per unitarea and L and W are the length and width of the channelmaterial, respectively. Then, the photocurrent of the hybrid

device could be expressed as

FIG. 2. Photodetector performance of

a SnS2 device before and after CIS

QDs deposition. (a) The measured I-V

curves with or without light illumina-

tion. Inset: AFM of the pristine device.

(b) Photoresponse under illumination

with different incident power. (c) The

calculated responsivity as a function of

incident power. (d) The time-resolved

photoresponse showing the rise and

decay time less than 110 ms.



02:49:46

Iph ¼W

LlCoxVDDVT : (4)

Substitute Equation (4) into Equation (1), the responsivity

could be expressed as

Rk ¼ aW

LlCoxVDP

b�1: (5)

Fig. 4(b) shows the responsivity of our hybrid device

as a function of light illumination, which fits very well

with Equation (5). According to our experimental results,

b� 0.48 is higher than that of a PbS-graphene hybriddevice.19 In general, the value of b indicates the efficiency ofcharges transfer from the layer of QDs to the channel mate-

rial. It depends on the quality of interface between the CIS

QDs layer and SnS2 NSs, the surface ligand used to prepare

QDs solution, and the experimental process.39 Therefore, by

carefully choosing the ligand and improving the experimen-

tal procedure, it is possible that the value of b and theresponsivity of the hybrid device could be further improved.

In summary, a hybrid device with sensitive photores-

ponse, fast response time, and improved responsivity was

fabricated by spin-coating CIS QDs layer onto the surface of

SnS2 NSs. These improvements benefit from strong light

absorption of CIS QDs and the type II heterojunction formed

between SnS2 surface and CIS QDs. As a result, the photo-

currents are enhanced by more than one order and the

responsivity of the hybrid device is higher than 600 A/W.

Besides, the experimental data of the responsivity at varied

power of incident illumination agree very well with the theo-

retical equation. Our work may broaden the 2D-0D system

and offer a method to improve the performance of optoelec-

tronic devices based on LMDs.

This work was supported by the National Natural Science

Foundation of China (Nos. 21373065 and 61474033), 973

Program of the Ministry of Science and Technology of China

(No. 2012CB934103), Beijing Natural Science Foundation

(No. 2144059), and CAS Key Laboratory of Nanosystem and

Hierarchical Fabrication. The authors gratefully acknowledge

the support of the K. C. Wong Education Foundation.

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