Journal of Alloys and Compounds 1017 (2025) 179201

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Journal of Alloys and Compounds

journal homepage: www.elsevier.com/locate/jalcom

Flexible self-powered ultraviolet photodetector based on the GQDs: Zinc

oxide nanoflower heterojunction
Yiming Liu , Xinsheng Tang , Ruxangul Jamal , Tursun Abdiryim * , Feng Xu ,
Nawrzhan Serkjan , Yajun Wang
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi, Xinjiang 830017, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: In this study, we present a flexible UV photodetector with a PET/ITO/GQDs: ZnO/PEDOS/ITO/PET structure,
Flexible UV PD utilizing ZnO nanoflowers (ZnO NFs) which are more suitable for flexible devices. The close contact between the
ZnO NFs petal-like ZnO flakes helps maintain the integrity of the ZnO layer and mitigate cracking issues, while Graphene
PEDOS
quantum dots (GQDs) fill the gaps between ZnO NFs, providing structural support and improving bending sta­
P-n heterojunction
Piezoelectric photoelectronic effect
bility. Additionally, Se atoms in the PEDOS structure and oxygen-rich functional groups at the edges of GQDs
interact with oxygen vacancies on the ZnO NFs surface, enhancing electron transport and further improving
device performance. This flexible photodetector shows a high responsivity of up to 2.23 mA/W under room
temperature and 0 V external bias (365 nm), with a detectivity of 1.949 × 1010 Jones, and response times of
0.074 s and 0.082 s. The device demonstrates good light response under different bending angles and after
multiple bending cycles, maintaining its detection capability even after 1000 bends, with a responsivity of
1.02 mA/W and a detectivity of 9.930 × 109 Jones. This indicates that the device possesses excellent flexibility
and stability.

1. Introduction polytetrafluoroethylene (PTFE), carbon cloth [14], polyester fiber [15],

mica [16], and paper substrates [17]. For example, Trung et al. [18]
UV detectors are devices that convert incident UV radiation into demonstrated a UV photodetector based on a 3D micropatterned
electrical signals and find applications in fields such as missile guidance, stretchable substrate with PbS quantum dots (QDs) and ZnO nanorods
ultraviolet communication, skin detection, flame detection, and pollu­ (NRs) as the optical sensing layer, which is responsive to UV, visible, and
tion monitoring [1,2]. To perform effectively in demanding environ­ near-infrared light.
ments, these detectors require increasingly advanced functionalities. ZnO, GaN, TiO₂, SnO₂, and similar materials are commonly used in
However, traditional UV detectors, which are often made on rigid sub­ UV photodetectors due to their broad responsiveness to specific ultra­
strates like monocrystalline silicon, quartz, and sapphire, are susceptible violet light wavelengths. Among these, ZnO is notable as a typical
to brittleness and breakage under bending or mechanical stress. This broadband semiconductor with a bandgap of 3.37 eV, which corre­
fragility limits their usability in challenging conditions [3,4]. sponds to the ultraviolet region of the spectrum [17,19–23]. ZnO offers
Flexible UV detectors offer excellent photoelectric properties and excellent electrical properties, low toxicity, high UV absorption coeffi­
present unique advantages, including being lightweight, impact- cient, good stability, strong visible light transmittance, and effective
resistant, and capable of withstanding significant deformations such as absorption in the ultraviolet range. In addition, ZnO has pyroelectric
stretching, compression, and bending [5]. These characteristics make effect and piezoelectric photoelectric effect, which will cause the device
them highly suitable for flexible wearable sensors with considerable to exhibit better performance under bending conditions. ZnO has a high
development potential [6]. Currently, flexible substrates used in UV piezoelectric constant compared to piezoelectric semiconductors such as
detectors include materials such as polyimide (PI) [7], polyethylene GaN, ZnS and InN [24–26]. This makes ZnO an ideal choice for flexible
naphthalate (PEN) [8,9], polyethylene terephthalate (PET) [10,11], UV PDs [27,28]. However, ZnO materials can have inherent surface
polyvinyl alcohol (PVA) [12], polydimethylsiloxane (PDMS) [13], imperfections that lead to longer response times, low dark currents, and

* Corresponding author.
E-mail address: tursunabdir@sina.com.cn (T. Abdiryim).

https://doi.org/10.1016/j.jallcom.2025.179201
Received 21 October 2024; Received in revised form 9 February 2025; Accepted 12 February 2025
Available online 13 February 2025
0925-8388/© 2025 Elsevier B.V. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

reduced responsivity. For instance, Yang et al. [17] developed a UV 2. Experimental section
photodetector using ZnO and polyethylene glycol (PEG) composites on
A4 paper, which achieved a response rate of 177 mA/W. Despite this, the 2.1. Growth of ZnO nanoflowers
extended rise time of 15 seconds limits its practical applications.
To address the challenges mentioned, strategies such as doping ZnO was deposited onto a flexible ITO/PET substrate using the I-T
modification, surface treatment, and the construction of p-n hetero­ mode technique. A 0.1 M zinc nitrate solution in distilled water was used
junctions are commonly employed. Initially, an organic-inorganic p-n as the electrolyte. During the electrochemical polymerization process,
heterojunction is created to establish an inherent electric field. This field ITO/PET, platinum, and Ag/AgCl served as the working, counter, and
facilitates the rapid separation of electron-hole pairs generated by reference electrodes, respectively, within a three-electrode electro­
photoexcitation, directing them towards opposite ends and thereby chemical cell controlled by electrochemical instrumentation (CHI760E).
enhancing both photocurrent and response time. Common p-type The I-T mode parameters were set to a voltage of − 0.75 V for a duration
organic semiconductor materials used in these applications include of 2700 seconds. After deposition, the ITO/PET substrate coated with
polypyrrole (PPy) [29], poly(3,4-ethylenedioxythiophene) (PEDOT) ZnO was rinsed with distilled water and air-dried [43]. Details of the
[30,31], polyaniline (PANI) [32], and poly(3,4-ethylenedioxyselenium) preparation and polymerization process of EDOS are provided in the
(PEDOS) [33], Shahruz et al. [34] successfully fabricated a PANI/ZnO supporting information (SI) and Fig. S1.
heterojunction UV photodetector, which operates at zero bias and
demonstrates reproducible and remarkable photoresponsivity. The de­ 2.2. Preparation of GQDs and GQDs: ZnO
vice exhibits high photocurrent, long-term stability, substantial UV
on/off switching capability, and low rise and fall times. PEDOS and its In the described procedure, 0.03 g of pitch carbon fibers were added
derivatives offer several advantages due to their low redox potential, to a solution of 2 mL HNO3 and 6 mL concentrated H2SO4. The mixture
electrochromism, charge transport properties, and narrow bandgap. was then agitated and sonicated at 80◦ C for two hours. After cooling, the
With an optical bandgap of 1.4 eV, PEDOS can accommodate more solution was diluted with 80 mL of deionized water, and the pH was
charge when doped compared to thiophene analogs, due to its lower adjusted to 8 by adding Na2CO3. The resulting solution, with a molec­
redox potential. Additionally, the polarizability of selenium atoms en­ ular weight of 1000 Da, was dialyzed in a dialysis bag for three days
hances charge transport through intermolecular selenium-selenium in­ [34]. UV excitation photos of the prepared GQDs are shown in Fig. S2.
teractions [35–37]. By forming a p-n heterojunction with ZnO, PEDOS Following the production of GQDs, the solution containing the GQDs
can effectively reduce surface defects and oxygen vacancies in ZnO, was spin-coated onto the ZnO/ITO/PET surface and then dried in an
resulting in a flexible UV detector with improved responsiveness and oven at 60◦ C for two hours.
shortened response times while maintaining self-powered detection
capabilities [38]. 3. Results and discussion
In addition, surface modification was employed to enhance the
performance of ZnO NFs. Quantum dots are quasi-zero-dimensional The device preparation process is illustrated in Fig. 1(a). Two flexible
nanostructures, typically spherical, with all three dimensions ITO/PET substrates are used for the growth of ZnO nanofibers (NFs) and
measured in nanometers. This structure provides them with unique PEDOS. After the film is formed, GQDs are spin-coated onto the ZnO NFs
advantages in optoelectronics. Among these, graphene quantum dots layer. The two substrates are then laminated together with their faces in
(GQDs) are composed of one or more layers of graphene sheets with contact, and a PVA layer is wrapped around them to create the test
lateral dimensions of less than 10 nm. GQDs exhibit excellent electronic, device. A p-n heterojunction is established between the ZnO (n-type)
thermal, and mechanical properties and are widely used in applications and PEDOS (p-type) layers. The integrated electric field formed by the
such as solar cells, supercapacitors, and biosensors [39,40] The GQDs ZnO-PEDOS junction swiftly releases photogenerated carriers, reducing
are dispersed as photosensitizers inside the ZnO NFs sheet layer, and the impact of defects on the ZnO NFs surface and improving device
co-generate photogenerated carriers with ZnO NFs during UV irradia­ operation. The incorporation of GQDs increases the number of photo­
tion to enhance the photocurrent of the device. Meanwhile, after the generated carriers, enhancing the device’s performance. Additionally,
device is bent, the introduction of GQDs can reduce the generation of GQDs support the ZnO NFs layer, helping to maintain the structural
cracks in the ZnO layer to a certain extent, or bridge the electron integrity of the ZnO film during bending and reducing the occurrence of
transport in the cracks. [41] Yin et al. [42] have presented a flexible UV cracks. The PVA wrapping enhances the cohesion between the two
photodetector based on GQDs@ZnO NWs. The integration of GQDs layers and minimizes carrier spillover, ensuring high efficiency of the
improves the device sensitivity by a factor of three and shortens the device under UV light irradiation.
response time by a factor of four. Analyzing the morphological characteristics of electrochemically
In this study, we designed a flexible self-powered UV PD featuring a grown ZnO nanofibers (NFs) and the incorporation of GQDs, as shown in
ZnO NFs structure modified with GQDs, combined with PEDOS to form a the subsequent figures, provides additional insight. In Fig. 1(b), the SEM
p-n heterojunction. The Se atoms in the PEDOS structure and the image of ZnO NFs reveals a uniform structure with petal-like formations
oxygen-rich functional groups at the edges of the GQDs interact with the in close contact, some of which are stacked. This configuration creates
oxygen vacancies on the ZnO NFs surface, resulting in excellent per­ an efficient pathway for electron transport. Furthermore, the petal-like
formance of the device in its unbent state. Under room temperature and three-dimensional structure increases the surface area exposed to
0 V external bias (365 nm), the device achieves a maximum responsivity light, enhancing UV light absorption and, consequently, the photocur­
of 1.86 mA/W, a maximum detectivity of 1.96 × 1010 Jones, and optimal rent of the UV detector. Fig. 1(c) presents a high-resolution TEM (HR-
rise/fall times of 0.082/0.084 s. The close contact between the ZnO TEM) image of ZnO, showing lattice stripe spacing of 0.27 nm, consis­
plate-like "petals" helps maintain the integrity of the ZnO layer and tent with literature reports [39]. Fig. S3 displays a TEM image of ZnO
alleviate cracking issues, while GQDs fill the gaps between the ZnO NFs NFs that illustrates their structural arrangement, which facilitates the
layers, providing higher bending stability during bending. The flexible transfer of photogenerated carriers between layers. This design allows
photodetector shows a response speed of up to 2.23 mA/W, a detectivity UV light that is not absorbed by the ZnO monolayer to pass through to
of 1.949 × 1010 Jones, and response times of 0.074 s and 0.082 s under subsequent layers, thereby improving the sensitivity of the UV detector.
60◦ bending conditions. The device maintains excellent light response Additionally, Fig. 1(d) shows the HR-TEM image of GQDs within ZnO
even after 1000 bending cycles, with a responsivity of 1.02 mA/W and a NFs. The GQDs, with particle sizes around 5 nm, are embedded within
detectivity of 9.930 × 109 Jones, demonstrating its outstanding flexi­ the ZnO NFs layer, ensuring their effective role as photosensitizers in the
bility and stability. device. Fig. 1(e) presents the SEM image of electrochemically

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

Fig. 1. (a) Schematic flowchart for manufacturing UV PD. (b)SEM of ZnO NFs grown on flexible ITO/PET. (c) HR-TEM showing the d spacing of the ZnO NFs. (d) HR-
TEM of GDQs: ZnO NFs. (e) SEM of PEDOS. (f) Mapping of GQDs: ZnO NFs. (g)EDS of GQDs: ZnO NFs. (h) UV–vis of ZnO NFs, GQDs: ZnO NFs. (i)Infrared spectrum of
ZnO NFs, GQDs: ZnO NFs. (j) XRD of GDQs: ZnO NFs.

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

polymerized PEDOS, revealing a flat layer with a uniform texture UV–visible absorption spectra in Fig. 1(h) show absorption peaks around
composed of small particles. This surface topology enhances the contact 350 nm for both ZnO NFs before and after GQD loading[44]. However,
between PEDOS and the ZnO NFs, improving device performance. the peaks are significantly higher after GQD incorporation, indicating an
Elemental mapping in Fig. 1(f) and EDS analysis in Fig. 1(g) show a enhanced UV absorption effect. Fig. 1(i) displays the infrared spectrum
uniform distribution of elements, with carbon content at 0.9 %, con­ of ZnO NFs with and without GQDs. Peaks around 700 cm⁻¹ correspond
firming the consistent loading of GQDs onto the ZnO substrate. The to the flexible substrate, while peaks at 1019 cm⁻¹ , 1246 cm⁻¹ , and

Fig. 2. (a) XPS full spectrum of ZnO NFs, GQDs: ZnO NFs. (b) Zn 2p of ZnO NFs, GQDs: ZnO NFs. (c) O 1 s, of ZnO NFs, GQDs: ZnO NFs. (d) C 1 s of ZnO NFs, GQDs:
ZnO NFs. (e) schema of UV PD.

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

1723 cm⁻¹ are attributed to C-O, C-H, and C– –O groups, respectively. configuration. Additional peaks at 287.69 eV and 285.37 eV correspond
These peaks indicate the presence of oxygen-containing functional to carbon-oxygen double and single bonds, respectively, confirming the
groups in the GQDs, which result from the oxidation step and facilitate presence of carbon bonds in the GQDs: ZnO NFs [47,48]. Fig. 2(e) il­
their solubility in water. Finally, Fig. 1(j) shows the XRD patterns of ZnO lustrates the interactions between GQDs: ZnO/PEDOS, where the
NFs with peaks at 31.73◦ , 34.34◦ , 36.29◦ , 47.41◦ , 56.45◦ , 62.82◦ , oxygen-containing groups at the edges of GQDs can fill the oxygen va­
66.50◦ , 67.76◦ , and 68.97◦ , corresponding to ZnO planes (100), (002), cancies on the ZnO surface while forming hydrogen bonds with the O
(101), (102), (110), (103), (200), (112), and (201). These patterns align atoms in the PEDOS structure. Additionally, the π-bonds of GQDs stack
with the standard spectrum (No. 00–036–1451) [45] and confirm the with the π-bonds in the PEDOS structure, creating π-π stacking. Conse­
hexagonal fibrillar zincite crystal structure of the ZnO NFs. quently, GQDs bridge the electronic transport between ZnO and PEDOS,
X-ray photoelectron spectroscopy (XPS) was used to examine the leading to a UV PD with enhanced photoresponse and shorter response
oxidation state and chemical composition of ZnO NFs. Fig. 2(a) displays times.
the full XPS spectra of ZnO NFs and GQDs: ZnO NFs, revealing the In order to study the optoelectronic performance of the flexible de­
presence of Zn (Zn 2p), O (O 1 s), and C (C 1 s) components. The Zn 2p vice, the working area as well as the light-exposed area of the flexible
spectra in Fig. 2(b) show two peaks at 1043.90 eV and 1020.82 eV, device was defined as shown in Fig. S4, and the light-exposed area of the
corresponding to Zn 2p₁/₂ and Zn 2p₃/₂, respectively, indicating a + 2 flexible device was 0.24 cm2. The current-voltage characteristics of the
oxidation state. The energy difference between these peaks is 23 eV, device under different light intensities with 365 nm wavelength light
consistent with literature values [24]. Compared to pristine ZnO NFs, were investigated, as shown in Fig. 3. Fig. 3(a) presents the I-T curve for
the peaks for Zn 2p₁/₂ and Zn 2p₃/₂ in GQDs: ZnO NFs show a 0.3 eV shift the pure ZnO/ZnO device. Although this device shows a relatively
to higher binding energies, suggesting an interaction between ZnO and typical response waveform, the photocurrent only reaches approxi­
GQDs. Fig. 2(c) shows the O 1 s spectra for ZnO NFs and GQDs: ZnO NFs, mately 7 nA within 10 seconds of UV irradiation and does not achieve its
with peaks observed at 530.69 eV. These peaks are attributed to the O²⁻ maximum equilibrium value. Furthermore, as illustrated in Fig. 3(b), the
ions within the ZnO lattice, and the differences between them are likely single ZnO device exhibits both an extended response time and a low
due to the interaction between GQDs and ZnO [46]. Similarly, the C 1 s photocurrent. In contrast, Fig. 3(c) illustrates the I-T curve for the PET/
spectra in Fig. 2(d) reveal significant peaks, ITO/ZnO/PEDOS/ITO/PET device, which displays a notably typical and
with the main peak at 283.88 eV indicating C-C bonds in the sp² well-defined response waveform. This device shows a stabilized

Fig. 3. The I-T curve and response time of the device (a), (b) ZnO/ZnO. (c), (d) ZnO/PEDOS. (e), (f) GQDs: ZnO/PEDOS. (g) shows the I-T curves of GQDs: ZnO/
PEDOS at different light intensities.

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

photocurrent of about 50 nA within 10 seconds of UV irradiation. Due to

Ilight − Id
the pyroelectric effect of the ZnO material [49], an abrupt output cur­ R= (1)
PS
rent is observed in the initial stages of UV irradiation, as shown in Fig. 3
(d) at stage I. This immediate current results from the combined influ­ Where Ilight is current during UV irradiation, Id is current in dark con­
ence of photoelectric and pyroelectric effects, referred to as Ipyro+photo. ditions, S is the portion of the device that is truly exposed to UV light,
Stage II in Fig. 3(d) demonstrates the stabilization of temperature and P is the light intensity.
changes on the ZnO surface following continued UV irradiation. During The detection rate (D*) is calculated as follows:
this phase, photogenerated electron pairs are converted into both pho­
toelectric and thermal effects, resulting in a stabilized output current R
D∗ = (2)
denoted as Iphoto+thermo. After the UV irradiation stops, the device’s (2eId /S)1/2
response rapidly declines to the dark current within a short period,
eventually stabilizing, as depicted in stages III and IV of Fig. 3(d). The Where e is a primary charge.
inclusion of PEDOS significantly reduces the response time of the device The performance of the device under varying light intensities is
compared to pure ZnO UV photodetectors, with rise and fall times of illustrated in Fig. S7. Fig. S7(a) shows how both the maximum output
0.166/0.168 seconds. This improvement is due to PEDOS acting as an current and the maximum smooth current of the GQDs: ZnO/PEDOS
excellent hole-transporting layer, which facilitates rapid hole movement device fluctuate with different light intensities. It is evident that as the
and forms a p-n heterojunction with ZnO, enhancing the separation of light intensity increases, the photocurrent also increases. This increase
electron-hole pairs generated by the photoelectric effect. This greatly in Ipyro+photo. Ipyro+photo is more pronounced due to the enhanced py­
shortens the device’s response time. The I-T curves for the PET/I­ roelectric effects of ZnO and GQDs at higher light intensities. Fig. S7(b)
TO/GQDs: ZnO/PEDOS/ITO/PET device, shown in Fig. 3(e), reveal that depicts the relationship between responsivity and light intensity. Ac­
the device continues to exhibit typical waveform behavior even with the cording to Eq. (1), responsivity is inversely proportional to light in­
addition of GQDs. However, the presence of GQDs results in a smoother tensity, which is generally reflected in the curve shown in Fig. S7.
waveform, with the smoothed current reaching approximately 115 nA However, the maximum responsivity of 1.91 mA is observed at
after 10 seconds of UV irradiation. Additionally, due to the thermal ef­ 0.56 mW/cm². This anomaly can be attributed to the improved contact
fect of GQDs under UV irradiation, the device demonstrates a stronger of the device during this specific test, which results in a reduced dark
pyroelectric effect compared to ZnO/PEDOS alone. As shown in Fig. 3 current and consequently an increased responsivity. demonstrates the
(f), the sharpness of Ipyro+photo is enhanced, resulting in a smoother correlation between detection rate and light intensity. According to Eq.
output current. The photogenerated electron-hole pairs at the GQDs, (2), D* is proportional to responsivity (R), and the data in Fig. S4
aided by the formation of a p-n heterojunction between ZnO NFs and confirm this relationship. Fig. S7(d) presents the link between response
PEDOS, undergo rapid separation, leading to rise and fall times of time and light intensity. The rise time is defined as the duration required
0.165/0.149 seconds, respectively. Finally, the device’s response to for the current to increase from 10 % to 90 % of the maximum photo­
varying light intensities was evaluated, with results displayed in Fig. 3 current, while the fall time is the time needed for the current to decrease
(g). The smooth current of the device increases gradually with rising from 90 % to 10 % of the maximum photocurrent. The figure shows a
light intensity, accompanied by a corresponding increase in its general decrease in response time with increasing light intensity, except
maximum output current. This is attributed to the enhanced visibility of for a minor increase at 2.40 mW/cm². This indicates that, within a
the pyroelectric effects of both ZnO and GQDs at higher light intensities. certain range, increasing light intensity helps reduce the device’s
Additionally, the reverse pyroelectric effect occurs when UV light dis­ response time. However, at excessively high light intensities, the
appears. The I-t curves of the ZnO/GQDs: ZnO devices are shown in increased number of photogenerated carriers can reduce the efficiency
Fig. S5. Fig. S5(a) shows the I-t curve of ZnO/GQDs: ZnO under UV of carrier separation in the p-n heterojunction, thereby increasing the
irradiation at 365 nm, 0.32 mW/cm2. It can be seen that the photocur­ response time Fig. S8 displays the dark current of the device. It shows
rent of the device is enhanced by the introduction of GQDs, but the that the dark current is significantly lower at 0.56 mW/cm² compared to
response time is still very long, and the photocurrent does not reach the other light intensities, resulting in a larger responsivity (R) at this
maximum value at an irradiation period of 10 s. The photocurrent of the intensity.
ZnO device is also enhanced by the introduction of GQDs. Fig. S5(b) To evaluate the performance of the flexible UV detector under
shows the I-t curves of ZnO/GQDs: ZnO at 365 nm, 0.32 mW/cm2 UV bending conditions, the ties of disposable medical masks were attached
irradiation, and 0.1 V bias voltage, in comparison, the photocurrent is to the upper and lower ends of the UV detector, as shown in the bending
greatly improved, but the response time is still very long. It can be seen schematic illustrated in Fig. 4. Fig. 4(a), (d), and (g) display physical
that constructing p-n heterojunction is the most effective means to views of the flexible device at different bending angles, and tests were
reduce the response time of the device. Fig. S6 shows the I-V curve of the conducted under these conditions. Fig. 4(b) shows the I-T curves of the
ZnO/ZnO, GQD: ZnO/ZnO (Fig. S6(a)), ZnO/PEDOS, and GQD: ZnO/­ UV detector under 365 nm, 0.32 mW/cm² UV irradiation at a 60◦
PEDOS (Fig. S6(c)) devices, and in order to see the current character­ bending angle, while Fig. 4(e) and (h) present the I-T curves for the same
istics of the devices more clearly at 0 V bias, the curves are enlarged in light intensity at 90◦ and 120◦ bending angles, respectively. From the
the range from − 0.05 V to 0.05 V, as shown in Fig. S6(b, d). It can be comparison of these graphs, it is evident that the photocurrent (Ipyr­
o+photo) decreases with increasing bending angle: at 60 bending, Ipyr­
◦
clearly seen that the current values of the two devices without PEDOS
are almost 0 at 0 V bias, indicating that the ZnO/ZnO and GQD: o+photo is 162.35 nA; at 90 ◦
, it is 109.53 nA; and at 120◦
, it is 83.25 nA.
ZnO/ZnO devices do not form a p-n heterojunction and do not have Despite this decrease, the device still exhibits a typical and repeatable
self-powered characteristics. In contrast, the current values of the waveform at each bending angle, indicating that the UV detector
ZnO/PEDOS and GQD: ZnO/PEDOS devices at 0 V bias are 0.17 and maintains its detection performance even at a 120◦ bending angle and
0.25 μA, respectively, demonstrating that the ZnO and PEDOS form a p-n demonstrates good flexibility and stability. The bending performance of
heterojunction, which gives the devices self-powered characteristics. the device without GQDs is shown in Fig. S9. At a 60◦ bending angle, the
Where the introduction of GQDs enhances the current values of the device maintains a normal response waveform, but the photocurrent is
devices. relatively low at around 30 nA. At bending angles of 90◦ and 120◦ , the I-
Some performance parameters of the device have been calculated T curve becomes irregular, and the photocurrent drops to approximately
[50,51]. It is how the responsivity (R) is calculated: 0.5 nA. This is due to the rigidity of the ZnO NFs film, which tends to
crack at larger bending angles. As shown in Fig. S10, significant cracking
appeared on the ZnO nanofibers (NFs) layer after the bending

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

Fig. 4. Bending morphology of UV PDs and their IT curves under bending conditions. (a), (b), (c) 60 ◦ bending. (d), (e), (f) 90◦ bending; (g), (h), (i) 120 ◦ bending.

performance test (see panels (a) and (b)). In Fig. S10(c), cracks indicating better performance compared to the unbent state.
measuring up to 197 nm are visible, supporting this observation. These To further examine the device’s performance under bending condi­
cracks obstruct electron transport, leading to a decrease in photocurrent tions, we compared the I-T curve at various bending angles with the I-T
and device instability. In contrast, in the GQDs: ZnO/PEDOS device, curve of the device in a flat, unbent state under the same illumination, as
GQDs are incorporated into the ZnO NFs layer, with many small spheres shown in Fig. 5(a). The device exhibits an increase in Ipyro+photo during
uniformly dispersed throughout. This dispersion reduces the formation 60◦ bending. At small bending angles, the two layers are in closer con­
of cracks and helps to bridge existing cracks, improving electron trans­ tact, and the PEDOS layer significantly enhances the performance of the
mission. As a result, the device performs better under bending condi­ ZnO layer. This improvement is attributed to the device’s assembly
tions Additionally, ZnO’s high piezoelectric constant allows the device method. The UV photodetector (PD) uses a flexible substrate, and during
to regulate the energy band structure at the contact junction interface the face-to-face lamination process, some gaps inevitably form. Wrap­
through piezoelectric polarization charges generated by external strain. ping the device with PVA helps prevent these gaps from widening during
This regulation helps control carrier generation, separation, transport, use and reduces carrier spillover.
and recombination, mitigating the impact of cracking in the ZnO film In addition, due to the piezoelectric photoelectric effect of ZnO, the
during bending. The performance parameters of the flexible device at device experiences a certain pressure when bent, which generates
different bending angles were calculated according to formulas (1) and piezoelectric polarization charges that increase the number of carriers.
(2), as shown in Fig. S11. The testing conditions were 0.32 mW/cm2, 0 V These two effects make the flexible device more suitable for operation
bias, and room temperature. Fig. S11(a) shows the photocurrent of the under small-angle bending. At small bending angles, the two layers in
flexible device under different bending conditions, where the photo­ face-to-face lamination adhere more closely to each other due to
current decreases with increasing bending angle. Similarly, the external forces, reducing the gap between them. However, as the
responsivity (Fig. S11(b)) and detectivity (Fig. S11(c)) follow the same bending angle increases, the area of the device exposed to light de­
trend. The response time (Fig. S11(d)) increases with the bending angle, creases, leading to a reduction in the carriers generated by the photo­
leading to a decrease in the device’s response speed. Under a 60◦ electric effect, pyroelectric effect, and piezoelectric photoelectric effect.
bending condition, the responsivity is 2.23 mA/W, the detectivity is Additionally, support from the GQDs diminishes over time, and the ZnO
1.949 × 1010 Jones, and the response times are 0.074 s and 0.082 s, and PEDOS films on the flexible substrate gradually develop cracks,

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

Fig. 5. (a) I-T curves at different bending angles. (b) I-T curves after different number of bends.

which impede carrier transmission and reduce the efficiency of carrier 1.86 mA/W, a maximum detection rate of 1.96 × 1010 Jones, and
transport. This results in a decrease in the combined pyroelectric and optimal rise/fall times of 0.082/0.084 s. Remarkably, even when bent
photoelectric current (Ipyro+photo) of the UV photodetector (PD) as the up to 120◦ , the photodetectors maintained their detection capabilities,
bending angle increases. Therefore, this UV PD is more suitable for with a maximum responsivity of 2.28 mA/W, a maximum detection rate
operation under small bending angles, making it more adaptable to of 1.95 × 1010 Jones, and optimal rise/fall times of 0.074/0.082 s.
complex working conditions and enhancing its practical significance. Furthermore, the devices demonstrated excellent mechanical durability,
Furthermore, the I-T curves of this flexible device were tested after retaining their detection activity after up to 1000 bends. Unlike many
various numbers of bending cycles. As depicted in Fig. 5(b), the device flexible counterparts that rely on applied voltage for optimal perfor­
was bent forward and backward at 90◦ and its I-T curves were measured mance, these devices exhibit remarkable performance even at zero bias
in the straightened state after 100, 500, 700, and 1000 bending cycles, voltage. Zhang et al. [41] designed a flexible UV photodetector based on
all under a test condition of 0.32 mW/cm². The results indicate that the silver nanowires, Ag NW@ZnO NR. Under a 5 V bias and 365 nm
device’s performance remains relatively stable with only minor fluctu­ (1.3 mW/cm2) UV light exposure, it exhibits excellent optical response
ations after bending cycles. However, after 1000 bending cycles, the with a responsivity of 6.5 μA/W and response times of 2.6 s and 2.3 s.
structures of ZnO and GQDs were damaged, leading to a decrease in Additionally, it demonstrates good flexibility and outstanding mechan­
temperature sensitivity. At the same time, large cracks appear in the ZnO ical stability after 1000 bending cycles.
layer after many bending cycles, affecting the transmission of photo­ Wu et al. [52] used borate polymers (BPs) as a co-substrate for the
generated carriers. With the combined effect of the two reasons, the photoactive layer substrate and conductive ink to construct an inte­
device loses the pyroelectric effect after 1000 bends. Overall, the GQDs: grated flexible UV photodetector. CuPc was chosen as the photoactive
ZnO/PEDOS device retains good UV detection activity even when bent component, and a high response rate of 32.7 μA/W was achieved at
and after multiple bending cycles. 365 nm illumination. The FPD device exhibited stable photoresponse
The performance of the devices developed in this research is during 2000 UV stimulations with continuous 50 % stretching. In
compared to various flexible UV photodetectors in Table 1. Notably, contrast, our PET/ITO/GQDs: ZnO/ITO/PET configuration demon­
these devices offer distinct advantages. Under the conditions of 365 nm strates superior practicality due to enhanced overall flexibility. The in­
wavelength, 0.32 mW/cm2 intensity, 0 V bias voltage, and room tem­ clusion of graphene quantum dots (GQDs) in the device structure not
perature, the photodetectors achieved a maximum responsivity of only improves flexibility but also offers advantages in response speed.

Table 1
Performance comparison of flexible UV photodetectors.
Photodetector Bias Voltage Wavelength (nm) R Rise time Fall time D*× 1010Jones Bending times Refs.
(mA/W)

FTO/CBINx/electrolyte/FTO-Pt 0V 365a 53.38 0.048 0.049 0.599 - [54]

PDMS/PEDOT: PSS/P3HT/PCBM/ZnO NPs − 1V 310b 510 34.9 24.9 - - [55]
TBVA-CuPc 0.2 V 365c 0.033 7.5 6.6 - 800 [52]
ZnO/Cu2O 0V 365d 0.98 0.0028 s 0.0025 s 186 - [53]
Ag NW@ZnO NR 5V 365e 0.0065 2.6 s 2.3 s - 1000 [20]
ZnS/SnO2 10 V 380 f 17.88 8s 61 s 25 500 [56]
TiO2/ Ti3C2Tx 5V 350 g 6 2.27 2.54 - 1000 [57]
PET/ITO/ZnO/PEDOS/ITO/PET 0V 365 h 0.61 0.081 s 0.091 s 0.5084 1000 This work
PET/ITO/GQDs: ZnO/PEDOS /ITO/PET 0V 365i 2.28 0.074 s 0.082 s 1.955 1000 This work

Light intensity: a-20 mW/cm2; b-47.46 μW/cm2; c-32.7 μW cm-2; d-3.3 mW/cm2; e-1.3 mW/cm2;
f-17.88 mW/cm2; g- 0.676 mW/cm2; h-0.32 mW/cm2; i-0.56 mW/cm2

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Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

This flexible device achieves self-powered detection with a response conduction band (CB) of ZnO. Simultaneously, these photogenerated
speed comparable to that of rigid devices [53,54] while ensuring high electron-hole pairs rapidly separate under the influence of the built-in
responsiveness. Further discussion on the flexibility aspect will be pro­ electric field formed by the p-n heterojunction of ZnO and PEDOS.
vided in the manuscript. The electrons migrate toward the ZnO side, while the holes migrate
Fig. 6 illustrates the operation mechanism of PET/ITO/GQDs: ZnO/ toward the PEDOS side and eventually accumulate on both sides of the
PEDOS/ITO/PET devices. Fig. 6(a) and (b) show the calculated values of ITO/PET interface. This process enables the ZnO-based UV detector to
the HOMO and LUMO levels of PEDOS, which are − 5.06 eV and respond quickly. Moreover, the addition of GQDs on the ZnO side allows
− 1.23 eV, respectively. The LUMO of PEDOS is significantly shifted by both materials to generate photoelectron pairs under UV irradiation,
3.27 eV from the conduction band (CB) of ZnO (-4.5 eV), providing which further enhances the photocurrent through efficient separation
sufficient driving force for the effective separation of photogenerated under the built-in electric field. The operation mechanism of the device
carriers and thereby enhancing the utilization of these carriers. The under bending conditions is shown in Fig. 6(f). When the device is bent
operation of the device under dark conditions is depicted in Fig. 6(c). In during use, stress is applied to the ZnO layer. This stress amplifies the
the absence of light, the photoelectronic effect of ZnO is minimal, photocurrent through the piezoelectric photoelectron effect, thereby
resulting in only a slight dark current that originates from the intrinsic improving the overall performance of the ZnO UV detector.
nature of the material itself. However, when exposed to UV radiation at Fig. 7(a) and (b) show the surface binding energies of GQDs-ZnO NFs
wavelengths equal to or greater than the band gap of ZnO, the photo­ and PEDOS-GQDs: ZnO. The binding energy between ZnO NFs and GQDs
electron effect (Fig. 6(d)) combines with the pyroelectric effect (Fig. 6 is − 8.19 eV, indicating a strong interaction and close contact between
(e)), leading to the formation of photogenerated electron-hole pairs. these components, which facilitates electron transfer between them. In
This occurs as electrons leap from the valence band (VB) to the contrast, the binding energy between PEDOS and GQDs: ZnO NFs is

Fig. 6. (a), (b)Theoretical calculation of HOMO and LUMO for PEDOS. Electron transport mechanisms of PET/ITO/GQDs: ZnO/PEDOS/ITO/PET devices (c) dark
conditions, (d) under ultraviolet light, (e) superimposed pyroelectric effect, (f) superimposed piezoelectric photoelectric effect.

9
Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

Fig. 7. (a) The binding energy of GQDs-ZnO NFs and (b) PEDOS-GQDs: ZnO, (c) the work function of ZnO NFs and (d) GQDs.

− 1.03 eV, suggesting the formation of a heterojunction structure that 4. Conclusion

generates an internal electric field, promoting the separation of photo­
generated electron-hole pairs. This mechanism endows the device with In summary, we have developed a flexible UV photodetector with a
self-powered characteristics and enhances the performance of the UV PET/ITO/GQDs: ZnO NFs/PEDOS/ITO/PET structure, which demon­
photodetector. strates excellent flexibility and stability, along with outstanding
However, the binding energy between PEDOS and GQDs: ZnO NFs is responsiveness and low response time. Due to the combined effects of
lower than that between GQDs and ZnO NFs, indicating reduced elec­ photoelectric, thermoelectric, and piezoelectric effects of ZnO, the de­
tron transfer capability between PEDOS and GQDs: ZnO NFs. Thus, vice exhibits remarkable UV photodetection capabilities. The p-n het­
when the device is bent at a small angle, electron transfer between them erojunction formed between PEDOS and ZnO, as well as the Se atoms in
becomes more efficient. This corresponds with the performance tests, the PEDOS structure and the oxygen-rich functional groups at the edges
where the flexible device shows better performance when bent at 60◦ of the GQDs interact with the oxygen vacancies on the ZnO NFs surface,
compared to its unbent state. Fig. 7(c) and (d) display the work functions enhance the photoelectric current and shorten the response time of the
of ZnO NFs and GQDs, where the work function is defined as the mini­ device. The close contact between the ZnO plate-like "petals" helps
mum energy required for an electron to move from the solid interior to maintain the integrity of the ZnO layer and alleviate cracking issues, at
its surface. The work function of ZnO NFs is 8.43 eV, while that of GQDs the same time, GQDs provide structural support to the ZnO layer,
is 5.99 eV. The lower work function of GQDs facilitates the generation of helping to maintain relative structural integrity during bending. Under
photogenerated electrons. Consequently, the addition of GQDs increases 365 nm UV light, 0 V bias voltage, and room temperature conditions,
the number of photogenerated carriers in the device, enhancing the UV the device achieves a maximum responsivity of 1.86 mA/W, a maximum
detection performance of the UV photodetector. This theoretically detectivity of 1.96 × 1010 Jones, and optimal rise/fall times of 0.082/
demonstrates that the introduction of GQDs can improve ZnO’s response 0.084 s. During bending, the maximum responsivity increases to
to UV light. 2.28 mA/W, the maximum detectivity is 1.95 × 1010 Jones, and the
rise/fall times are shortened to 0.074/0.082 s. At a 120◦ bending angle,
the device has a responsivity of 0.91 mA/W and a detectivity of
7.339 × 109 Jones. Even after 1000 bends at a 90◦ angle, the device

10
Y. Liu et al. Journal of Alloys and Compounds 1017 (2025) 179201

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Foundation of China (No. 52163020, No. 21865034) and the Xinjiang NW@ZnO NRs with high performance, J. Mater. Sci. Technol. 110 (2022) 65–72,
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