Piezophototronic Effect-Enhanced Highly Sensitive Flexible Photodetectors Based on Electrohydrodynamic Direct-writing Nanofiber Self-stacking

Abstract

Flexible photodetectors are ideal for short-range communication in lightweight microintegrated systems. However, low-bonding interface and high-power cost of photosensitive components greatly limit their application in flexible communication systems. To address this, herein, piezophototronic effect-enhanced sensing components are proposed for flexible photodetectors. This approach leverages the piezophototronic effect to modulate nanoscale charge transport and the precision of electrohydrodynamic direct-writing to achieve controlled nanofiber assembly, thereby enhancing interfacial bonding and overall device performance. By employing electrohydrodynamic direct-writing, a copper-ammonia complex ((Cu(NH₃))(CN)) nanofiber is self-stacked on a zinc oxide (ZnO) nanofiber to construct a zinc oxide and copper ammine complex (ZnO@(Cu(NH₃))(CN)) photodetector with low static power consumption and high responsiveness through the combined effects of piezoelectricity and fiber self-stacking. The dark current is reduced to 1.12 × 10⁻⁷ A, and the static power consumption of the photodetector is also decreased. The responsiveness is up to 13.3 A/W, with response and recovery times of 11 and 9 ms under ultraviolet (UV) light illumination, respectively, fulfilling the requirements for highly sensitive photodetection owing to the high interface bonding. The detector's threshold voltage is tunable, ranging from 6 V for 5 stacking layers to 20 V for 25 stacking layers, thereby allowing the device's performance to be precisely tailored to specific application requirements. Leveraging the exceptional optoelectronic performance of the ZnO@(Cu(NH₃))(CN) photodetector, this study expands the application scenarios of flexible photodetectors and demonstrates their potential in the fields of 6G technology and battlefield communication.

Keywords

Electrohydrodynamic direct-writing / Flexible photodetectors / Piezophototronic effect-enhanced / Self-stacking / Encrypted communication

References

[1] QuSD, LiuJQ, HuJH, SunL, XuWT. Flexible DPPT-TT/PEO fiber-exploiting electro-optical synaptic transistor for artificial withdrawal reflex arc. Adv Fiber Mater, 2024, 6401

[2] KyriacouGA. Oxide electronics for 5G and 6G. Nat Electron, 2021, 4705

[3] YangSP, MachariaDK, AhmedS, ZhuB, ZhongQP, WangHF, ChenZG. Flexible and reusable non-woven fabric photodetector based on polypyrrole/crystal violate lactone for NIR light detection and writing. Adv Fiber Mater, 2020, 2150

[4] WuY, ChenJ, WangY, YuanZ, HuangC, SunJ, FengC, LiM, QiuK, ZhuS. Tbps wide-field parallel optical wireless communications based on a metasurface beam splitter. Nat Commun, 2024, 157744

[5] ChenJX, OuyangWX, YangW, HeJH, FangXS. Recent progress of heterojunction ultraviolet photodetectors: materials, integrations, and applications. Adv Funct Mater, 2020, 3018

[6] WangF, ZouXM, XuMJ, WangH, WangHL, GuoHJ, GuoJX, WangP, PengM, WangZ, WangY, MiaoJS, ChenFS, WangJL, ChenXS, PanAL, ShanCX, LiaoL, HuWD. Recent progress on electrical and optical manipulations of perovskite photodetectors. Adv Sci, 2021, 815

[7] WuWT, LiLL, LiZX, SunJZ, WangLL. Extensible integrated system for real-time monitoring of cardiovascular physiological signals and limb health. Adv Mater, 2023, 359

[8] ZhuY, ChenHB, HanRM, QinH, YaoZY, LiuH, MaYF, WanXJ, LiGH, ChenYS. High-speed flexible near-infrared organic photodiode for optical communication. Natl Sci Rev, 2024, 1112

[9] ZhangDT, Fuentes-HernandezC, VijayanR, ZhangY, LiYZ, ParkJW, WangYY, ZhaoYH, AroraN, MirzazadehA, DoY, ChengTY, SwaminathanS, StarnerT, AndrewTL, AbowdGD. Flexible computational photodetectors for self-powered activity sensing. npj Flex Electron, 2022, 68

[10] PengMF, WenZ, SunXH. Recent progress of flexible photodetectors based on low-dimensional II–VI semiconductors and their application in wearable electronics. Adv Funct Mater, 2023, 3324

[11] WangP, LanYY, HuanCM, LuoJL, CaiWC, FanJT, HeXJ, HuangZF, ZhuL, KeQQ, ZhangGY, LinSH. Recent progress on performance-enhancing strategies in flexible photodetectors: from structural engineering to flexible integration. Mater Sci Eng R Rep, 2023, 15643

[12] SarkarK, DeviP, KimKH, KumarP. II–-V nanowire-based ultraviolet to terahertz photodetectors: sevice strategies, recent developments, and future possibilities. Trends Anal Chem (TrAC), 2020, 13018

[13] WuZ, WuYJ, YangLF, ZuoXC, WangZH, YanYK, LiWH, ChangDD, GuoYL, MoXL, LuXF, LiuYQ, ZhaoY. Template-assisted fabrication of single-crystal-like polymer fibers for efficient charge transport. Adv Fiber Mater, 2023, 52069

[14] ZhuXL, QiuH, ZhangY, ManZM, LuWY, BaoNZ, WuG. Vertical-aligned and ordered-active architecture of heterostructured fibers for high electrochemical capacitance. Adv Fiber Mater, 2024, 6312

[15] SimoneG, DysonMJ, MeskersSCJ, JanssenRAJ, GelinckGH. Organic photodetectors and their application in large area and flexible image sensors: the role of dark current. Adv Funct Mater, 2020, 3016

[16] XiongYT, ChenB, XuXZ, DaiSJ, ZhanYQ, XuXB. Facile fabrication of highly crystallized, air-stable, and flexible perovskite micromesh film photodetector. Adv Opt Mater, 2024, 1212

[17] TongSC, YuanJ, ZhangCJ, WangCH, LiuBX, ShenJQ, XiaHY, ZouYP, XieHP, SunJ, XiaoS, HeJ, GaoYL, YangJL. Large-scale roll-to-roll printed, flexible and stable organic bulk heterojunction photodetector. npj Flex Electron, 2018, 28

[18] TongSC, GongCD, ZhangCJ, LiuG, ZhangD, ZhouCH, SunJ, XiaoS, HeJ, GaoYL, YangJL. Fully-printed, flexible cesium-doped triple cation perovskite photodetector. Appl Mater Today, 2019, 15389

[19] MondalS, DuttaK, DuttaS, JanaD, KellyAG, DeS. Efficient flexible white-light photodetectors based on BiFeO₃ nanoparticles. ACS Appl Nano Mater, 2018, 1625

[20] LiL, HuCQ, ShenGZ. Low-dimensional nanostructure based flexible photodetectors: device configuration, functional design, integration, and applications. Acc Mater Res, 2021, 2954

[21] LeeYH, LeeSH, WonY, KimH, YangSJ, AhnJ, MunJ, LeeJH, DouLT, RhoJ, OhJH. Boosting the performance of flexible perovskite photodetectors using hierarchical plasmonic nanostructures. Small Struct, 2024, 511

[22] LiXY, ShaoCR, ZhaoYP, OuyangG, HuW, ZhangJF. Pyramid-shaped perovskite single-crystal growth and application for high-performance photodetector. Adv Opt Mater, 2024, 128

[23] ZhangC, TuXY, LuoYM, HaiYL, YaoX, XianKH, PenaTAD, LiY, LiYR, LiMJ, YeL, WuJY, FeiZP. Enhanced molecular planarity for high-performance photodetectors: Effect of backbone conformation via alkyl substitution position control in dithienoquinoxaline-based conjugated polymers. Chem Eng J, 2024, 48810

[24] LiZL, JoshiMK, ChenJX, ZhangZM, LiZQ, FangXS. Mechanically compatible UV photodetectors based on electrospun free-standing Y³⁺-doped TiO₂ nanofibrous membranes with enhanced flexibility. Adv Funct Mater, 2020, 3011

[25] ZhangSC, GeYL, QinX, WangXK, TaoT, YuLM, SongXH, JiangYR, XiaCX. Vacuum-assisted growth of single crystal perovskite arrays toward ultralow dark current photodetectors. Adv Funct Mater, 2024, 359

[26] ChenC, ZhaoYM, YuHL, JiaoXY, HuXG, LiX, HouPX, LiuC, ChengHM. High-performance infrared photodetector based on single-wall carbon nanotube films. Carbon, 2023, 206150

[27] ChenC, YuHL, ZhaoYM, HouPX, GuoSY, LiSQ, WangHZ, TaiKP, LiuC. Ultrahigh-response flexible photothermoelectric photodetectors based on a graded Bi2Te3-carbon 2 Te 3-carbon nanotube hybrid. Chem Eng J, 2024, 4978

[28] LiuP, DingEX, XuZY, CuiXQ, DuMD, ZengWJ, KarakassidesA, ZhangJ, ZhangQ, AhmedF, JiangH, HakonenP, LipsanenH, SunZP, KauppinenEI. Wafer-scale fabrication of wearable all-carbon nanotube photodetector arrays. ACS Nano, 2024, 1818900

[29] LeungSF, HoKT, KungPK, HsiaoVKS, AlshareefHN, WangZL, HeJH. A Self-powered and flexible organometallic halide perovskite photodetector with very high detectivity. Adv Mater, 2018, 308

[30] CaiS, XuXJ, YangW, ChenJX, FangXS. Materials and designs for wearable photodetectors. Adv Mater, 2019, 3115

[31] PengYY, LuJF, WangXD, MaWD, QueML, ChenQS, LiFT, LiuXH, GaoWC, PanCF. Self-powered high-performance flexible GaN/ZnO heterostructure UV photodetectors with piezo-phototronic effect enhanced photoresponse. Nano Energy, 2022, 949

[32] SuL, YanTT, LiuXY, CaoF, FangXS. A tunable polarization field for enhanced performance of flexible BaTiO₃@TiO₂ nanofiber photodetector by suppressing dark current to pA level. Adv Funct Mater, 2023, 339

[33] PoppleD, ShekhirevM, DaiCH, KimP, WangKX, AshbyP, HelmsBA, GogotsiY, RussellTP, ZettlA. All-liquid reconfigurable electronics using jammed MXene interfaces. Adv Mater, 2023, 358

[34] LiCC, LiX, LiuX, MaLD, YanH, TongL, YangZB, LiuJX, BaoDY, YinJK, LiXJ, WangP, LiR, HuangL, YuM, JiaST, WangT. On-substrate fabrication of CsPbBr₃ single-crystal microstructures via nanoparticle self-assembly-assisted low-temperature sintering. ACS Nano, 2024, 189128

[35] ZhangQF, LiQ, ChenRS, ZhangMY, FangWN, LiJX, WangMD, YunF, WangT, HaoY. Large-area self-assembled hexagonal boron nitride nanosheet films for ultralow dark current vacuum-ultraviolet photodetectors. Adv Funct Mater, 2024, 3413

[36] HeZR, BiS, Asare-YeboahK. Hybrid system of polystyrene and semiconductor for organic electronic applications. Processes, 2024, 1231

[37] LouZ, ShenGZ. Flexible photodetectors based on 1D inorganic nanostructures. Adv Sci, 2016, 319

[38] QiaoS, LiuJH, NiuXN, LiangBL, FuGS, LiZQ, WangSF, RenKL, PanCF. Piezophototronic effect enhanced photoresponse of the flexible Cu(In, Ga)S_e2 (CIGS) heterojunction photodetectors. Adv Funct Mater, 2018, 288

[39] ShiauJS, BrahmaS, HuangJL, LiuCP. Fabrication of flexible UV-B photodetectors made of Mg_xZn_1−xO films on PI substrate for enhanced sensitivity by piezophototronic effect. Appl Mater Today, 2020, 2010

[40] TangX, JiangHS, LinZL, WangX, WangWL, LiGQ. Wafer-scale vertical 1D GaN nanorods/2D MoS₂/PEDOT:PSS for piezophototronic effect-enhanced self-powered flexible photodetectors. Nano-Micro Lett, 2025, 1715

[41] SunJC, ZhangXW, LangYY, BianJM, GaoRX, LiPD, WangYX, LiCR. Piezo-phototronic effect improved performance of n-ZnO nano-arrays/p-Cu₂O film based pressure sensor synthesized on flexible Cu foil. Nano Energy, 2017, 3296

[42] DaiYJ, WangXF, PengWB, XuC, WuCS, DongK, LiuRY, WangZL. Self-powered Si/CdS flexible photodetector with broadband response from 325 to 1550 nm based on pyro-phototronic effect: an approach for photosensing below bandgap energy. Adv Mater, 2018, 308

[43] DuXX, TianWL, PanJH, HuiB, SunJH, ZhangKW, XiaYZ. Piezo-phototronic effect promoted carrier separation in coaxial p-n junctions for self-powered photodetector. Nano Energy, 2022, 929

[44] NamG-H, BaekS-H, ParkI-K. Growth of ZnO nanorods on graphite substrate and its application for Schottky diode. J Alloys Compd, 2014, 61337

[45] FuX-W, LiaoZ-M, ZhouY-B, WuH-C, BieY-Q, XuJ, YuD-P. Graphene/ZnO nanowire/graphene vertical structure based fast-response ultraviolet photodetector. Appl Phys Lett, 2012.

[46] CostasA, FloricaC, PredaN, BesleagaC, KuncserA, EnculescuI. Self-connected CuO–ZnO radial core–shell heterojunction nanowire arrays grown on interdigitated electrodes for visible-light photodetectors. Sci Rep, 2022, 126834

[47] GuoW, YangY, LiuJ, ZhangY. Tuning of electronic transport characteristics of ZnO micro/nanowire piezotronic Schottky diodes by bending: threshold voltage shift. Phys Chem Chem Phys, 2010, 1214868

[48] LiuX, GuLL, ZhangQP, WuJY, LongYZ, FanZY. All-printable band-edge modulated ZnO nanowire photodetectors with ultra-high detectivity. Nat Commun, 2014, 59

[49] DuX, ZhongY, KangG, JiangJ, WangX, LiW, ZhengG. Low-temperature self-stacking ink for electrohydrodynamic direct writing. ACS Appl Polym Mater, 2023, 55314

Funding

National Natural Science Foundation of China(52405424)

Science and Technology Programme of Fujian Province(2024J010011)

Shenzhen Science and Technology Plan Project(JSGG20220831094600002)

Scientific and Technological Plan Projects in Xiamen(2022CXY0101)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China