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Yuxiang Wang, Rikuto Suzuki, Tomoki Furukawa, Takahiro Kaneta, Ryohei Kameyama, Shun Watanabe, Kazuya Yamaguchi, Kosuke Suzuki, [Jun Takeya](https://orcid.org/0000-0002-7003-1350), [Yu Yamashita](https://orcid.org/0000-0001-7966-3197)

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[Multivalent oxide-cluster ion doping for functionalizing semicrystalline polymer semiconductors](https://mdr.nims.go.jp/datasets/1444b5f3-d79b-492a-a099-d4212ce4ee7f)

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Applied PhysicsExpress      LETTER • OPEN ACCESSMultivalent oxide-cluster ion doping forfunctionalizing semicrystalline polymersemiconductorsTo cite this article: Yuxiang Wang et al 2026 Appl. Phys. Express 19 081001 View the article online for updates and enhancements.You may also likeEffective Charge Transport in Poly(3,4-ethylenedioxythiophene) Based HybridFilms Containing Polyoxometallate RedoxCentersLidia Adamczyk, Pawel J. Kulesza,Krzysztof Miecznikowski et al.-Designing Polyoxometalate Thin Films onCarbon Nanomaterials forPseudocapacitive ElectrodesMatthew Genovese, Yee Wei Foong andKeryn Lian-Polyoxometalates As VersatileComponents for Hybrid Electrode andElectrolyte MaterialsPedro Gómez-Romero-This content was downloaded from IP address 144.213.253.16 on 02/09/2026 at 06:29https://doi.org/10.35848/1882-0786/ae8e2b/article/10.1149/1.1859710/article/10.1149/1.1859710/article/10.1149/1.1859710/article/10.1149/1.1859710/article/10.1149/MA2015-02/9/563/article/10.1149/MA2015-02/9/563/article/10.1149/MA2015-02/9/563/article/10.1149/MA2014-01/24/1048/article/10.1149/MA2014-01/24/1048/article/10.1149/MA2014-01/24/1048Applied Physics Express 19, 081001 (2026) LETTERhttps://doi.org/10.35848/1882-0786/ae8e2bMultivalent oxide-cluster ion doping for functionalizing semicrystalline polymersemiconductorsYuxiang Wang1,2, Rikuto Suzuki1, Tomoki Furukawa1, Takahiro Kaneta1, Ryohei Kameyama1, Shun Watanabe1,Kazuya Yamaguchi3, Kosuke Suzuki1,3, Jun Takeya1,2,* and Yu Yamashita1,2,*1Department of Advanced Materials Science, Graduate School of Frontier Sciences, The University of Tokyo, 5-1-5 Kashiwanoha, KashiwaChiba 277-8561, Japan2Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki305-0044, Japan3Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan*E-mail: takeya@k.u-tokyo.ac.jp and yamashita.yu@nims.go.jpReceived July 5, 2026; revised July 16, 2026; accepted July 21, 2026; published online August 7, 2026Molecular doping has enabled control of electronic properties in semiconducting polymers for studies of charge transport and device applications.However, conventional dopant anions are mostly organic monovalent species whose roles are largely limited to stable charge compensation.Here, we introduce polyoxometalates as multivalent oxide-cluster dopant ions into semicrystalline polymer semiconductors. In particular, filmsdoped with size-compatible divalent [W6O19]2− retain lamellar order, exhibit conductivity above 200 S cm−1, and show a Hall response, indicat-ing partially coherent carrier transport. Compared with inert-anion-doped films, [W6O19]2−-doped films show enhanced anodic response in theoxygen-evolution region, demonstrating functional multivalent-ion doping for electronic and electrocatalytic polymer semiconductor films. © 2026The Author(s). Published on behalf of The Japan Society of Applied Physics by IOP Publishing LtdSupplementary material for this article is available onlineMolecular doping, which introduces molecular dopantsinto semiconducting polymer films through redoxreactions, is a key strategy for controlling their elec-tronic properties.1) Solution-processable polymer semicon-ductors provide large-area and mechanically compliant thinfilms for electronic and optoelectronic devices, includingphotovoltaic cells,2, 3) organic thermoelectrics,4, 5) and cir-cuit elements such as transistors and diodes.6–9) In theseapplications, molecular doping can control carrier density,tune energy-level alignment, reduce contact resistance, andenable high electrical conductivity in polymer semiconductorfilms.Recent advances in ion-exchange and related doping strate-gies have expanded the accessible range of dopant ionsin semiconducting polymers.10–14) In ion-exchange doping,redox reactions first generate charged polymer chains withexchangeable counterions, which are subsequently replacedby dopant ions supplied from solution. Dopant-ion design hasbeen shown to affect doped-state stability, energetic disorder,microstructure, charge transport, thermoelectric performance,and the formation of highly crystalline doped thin films.15–17)These studies indicate that dopant ions are not merely passivecharge compensators; their size, charge density, and spa-tial arrangement can strongly influence the structure-propertyrelationships of doped polymer semiconductors. Recent stud-ies have shown that organic dopant dianions or dianioniccounterions can be incorporated into polymer semiconduc-tors, offering a route to dense charge compensation with fewercounterions.18, 19) Such multivalent dopant species can alsostrongly modulate the electronic states of doped polymers,including the promotion of bipolaron formation.20) However,dianion-dominated regimes have mainly been demonstratedat relatively low dopant fractions, with conductivities of onlya few S cm−1. This leaves room for new multivalent dopantions that combine dense charge compensation, structural com-patibility, and additional molecular functionality.Polyoxometalates (POMs) are promising candidates forfunctional dopant ions because they are multivalent oxide-cluster ions with tunable redox and catalytic properties.21–27)A Keggin-type POM, phosphomolybdic acid, has been usedfor solution-based p-doping of semiconducting polymers.3, 28)If incorporated as dopant ions in ordered polymer semicon-ductor films, POMs could provide dense multivalent chargecompensation while also introducing oxide-cluster-basedinterfacial functionality. A central challenge is that POMsare much larger and more highly charged than conventionalorganic monoanions. Their incorporation into semicrystallinepolymer semiconductors would disrupt lamellar packing anddeteriorate carrier transport if the dopant size is incompatiblewith the polymer nanostructure.29) Therefore, size-compatibledopant design is essential for introducing multivalent oxide-cluster ions into ordered polymer films without sacrificingsemicrystalline order.Here, we demonstrate the incorporation of POMsinto semicrystalline poly(2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene) (PBTTT) films by anion-exchange doping. Unlike larger Keggin-type POMspreviously used for polymer doping, the smaller Lindqvist-type [W6O19]2− anion is compatible with the PBTTTlamellar nanostructure, allowing divalent oxide-cluster ionsto be incorporated while preserving the ordered film structure.The resulting POM-doped PBTTT films exhibit electricalconductivity above 200 S cm−1 and show a Hall response,indicating partially coherent carrier transport in the organic–inorganic hybrid semiconductor film. As a demonstrationof interfacial electrochemical functionality, the POM-dopedContent from this work may be used under the terms of the Creative Commons Attribution 4.0 license. Any further distribution ofthis work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.081001-1© 2026 The Author(s). Published on behalf ofThe Japan Society of Applied Physics by IOP Publishing Ltdhttps://doi.org/10.35848/1882-0786/ae8e2bhttps://crossmark.crossref.org/dialog/?doi=10.35848/1882-0786/ae8e2b&domain=pdf&date_stamp=2026-8-7mailto:takeya@k.u-tokyo.ac.jpmailto:yamashita.yu@nims.go.jphttps://doi.org/10.35848/1882-0786/ae8e2bhttps://creativecommons.org/licenses/by/4.0/Appl. Phys. Express 19, 081001 (2026) Y. Wang et al.Fig. 1. Anion-exchange doping using POMs. (a) Illustration of [W6O19]2−-doped PBTTT. (b) Schematic of anion exchange from F4TCNQ•− to[W6O19]2−. (c) Optical absorbance spectra of PBTTT films before and after the treatment with dopant solutions. (d) Conductivity of pristine andF4TCNQ/TBA2[W6O19]-treated PBTTT films.films also show an enhanced anodic response in the oxygen-evolution region compared with PBTTT films doped with aninert molecular anion. These results highlight POM dopingas a versatile strategy for functionalizing semicrystallinepolymer semiconductors with multivalent oxide-cluster ions,opening opportunities to explore electronic transport andinterfacial electrochemical functionality in ordered hybridfilms.The progress of anion exchange doping was confirmedby UV–Vis–near-IR (NIR) absorption spectroscopy andconductivity measurements of PBTTT thin films (Figs. 1(c)and 1(d)). Spin-coated PBTTT films were immersed ina doping solution containing TBA2[W6O19] (TBA =tetra-n-butylammonium) and 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ). In the pristinePBTTT film, an absorption peak attributed to the π–π*transition appeared around 550 nm.30) After immersion inthe F4TCNQ solution, the intensity of this peak decreased,and new features emerged around 800 nm and in the NIRregion, consistent with p-type doping of PBTTT.10, 31, 32) Thepeaks at 730 and 830 nm are attributed to the F4TCNQ•−.When doping solutions containing F4TCNQ together witheither TBA2[W6O19] as the Lindqvist-type POM source orNa3[PW12O40] as the Keggin-type POM sourcewere used, thepeaks associated with F4TCNQ•− became negligible, whilethe spectral features of doped PBTTT remained. These resultsprovide strong evidence for the successful anion-exchangedoping of PBTTT with [W6O19]2− and [PW12O40]3−. For[PW12O40]3−, the Na+ salt was specifically employedbecause TBA salts did not enable efficient anion exchangeunder these conditions. The anion-exchange efficiency forvarious POMs is discussed in the Supplementary Information(Fig. S1). Conductivity measurements further support thisconclusion. The conductivity of the PBTTT thin film withthickness of 50 nm, increased from approximately 10−3 Scm−1 to 200 S cm−1 through this doping process (Fig. 1(d)).The introduced dopant anion was identified by X-ray pho-toelectron spectroscopy (XPS, Fig. 2(a)). While the pris-tine PBTTT thin film exhibited C 1s and S 2p peaks, O1s and W 4f peaks were observed after treatment with theF4TCNQ/TBA2[W6O19] solution. Under the employed dop-ing condition, the F 1s signal disappeared completely (Fig.S2), confirming nearly quantitative replacement of F4TCNQ-derived anions by the introduced POM species.Quantitative XPS analysis (Figs. 2(b)–2(d) and Table I)gave an incorporation ratio of one [W6O19]2− per 4.1 PBTTTmonomer units from the C/W atomic ratio. Because[W6O19]2− is dianionic, this composition corresponds toapproximately one hole per two PBTTT monomer units.This doping level is reasonable compared with F4TCNQ-doped PBTTT, where one hole is generated per approximatelythree monomer units.31) Anion exchange can shift the doping081001-2© 2026 The Author(s). Published on behalf ofThe Japan Society of Applied Physics by IOP Publishing LtdAppl. Phys. Express 19, 081001 (2026) Y. Wang et al.Fig. 2. XPS analysis of PBTTT thin films. (a) Wide-scan XPS spectra and narrow-scan spectra in the (b) W 4f, (c) S 2p, and (d) F 1s regions for pristineand F4TCNQ/TBA2W6O19-treated PBTTT thin films.Table I. XPS elements analysis of atomic concentration [%].C S W O F NPristine 92.4 7.2 — 0.4 — —TBA2W6O19-treated 80.9 5.6 2.8 10.8 — —equilibrium toward higher oxidation states compared withF4TCNQ doping,10) consistent with the higher doping levelobserved in our XPS and UV–Vis-NIR spectra. The W 4fpeak positions indicate that the incorporated tungsten speciesremain predominantly in the W(VI) state, consistent withincorporation of [W6O19]2− without significant reduction ordecomposition.Grazing-incidence wide-angle X-ray scattering (GIWAXS)measurements showed that PBTTT retains an edge-on ori-entation after doping with [W6O19]2− (Figs. 3(a)–3(c)). Thestructural parameters extracted from the line profiles aresummarized in Table II. Upon [W6O19]2− doping, the lamel-lar spacing increased, whereas the out-of-plane FWHM wasnearly unchanged (Fig. 3(e)), indicating that the lamellarorder was preserved. The in-plane peak shifted to higherqxy and slightly narrowed (Fig. 3(d)), suggesting a reducedπ-stacking distance and improved in-plane ordering.10, 31, 33)These results indicate that [W6O19]2− anions are mainlyincorporated into the alkyl side-chain regions without dis-rupting the conjugated backbone packing. In contrast, dopingwith the larger [PW12O40]3− anion caused substantial peakbroadening in both directions, indicating significant structuraldisorder.Carriers in semicrystalline PBTTT thin films doped with[W6O19]2− exhibit band-like transport characteristics, as evi-denced by Hall effect measurements. At 200 K, the Hallvoltage (VH) showed a linear dependence on the applied mag-netic field (Fig. 4(a)), confirming the presence of delocalizedcarriers. From linear fitting of the Hall voltage as a function ofmagnetic field (Fig. 4(b)), the carrier density and Hall mobil-ity at different temperatures were extracted. However, theHall mobility was only 0.26 cm2 V−1 s−1 (Fig. 4(c)), lowerthan that of F4TCNQ•− (1.8 cm2 V−1 s−1)31) or monoanion-doped (2.4 cm2 V−1 s−1) PBTTT.10) This reduced Hallmobility may arise from hopping carriers that partially sup-press the Hall voltage,34) likely because of electrostatic poten-tial fluctuations induced by the dianionic dopant ions. Notethat, in such a mixed transport regime, the Hall carrier den-sity is overestimated. Consistent with this interpretation, theoverall conductivity follows a variable range hopping (VRH)transport (Fig. 4(d)). The temperature-dependent conductiv-ity showed good agreement with the VRH model (Fig. S3),suggesting a hopping contribution exists. Together with theHall response described above, this result supports a mixedtransport picture in which band-like and hopping transportcomponents coexist in the [W6O19]2−-doped PBTTT film.081001-3© 2026 The Author(s). Published on behalf ofThe Japan Society of Applied Physics by IOP Publishing LtdAppl. Phys. Express 19, 081001 (2026) Y. Wang et al.Fig. 3. GIWAXS analysis of PBTTT. 2D GIWAXS patterns of (a) [W6O19]2−-doped , (b) [PW12O40]3−-doped, and (c) pristine PBTTT thin films.(d) In-plane (qxy) and (e) out-of-plane (qz) GIWAXS line profiles of pristine and doped PBTTT thin films.Table II. Structural parameters extracted from GIWAXS analysis of pristine and POM-doped PBTTT films.Lamellar distance (Å) Out-of-plane FWHM (Å−1) π-stacking distance (Å) In-plane FWHM (Å−1)Pristine 21.4 0.011 3.65 0.095[W6O19]2−-doped 24.9 0.012 3.52 0.070[PW12O40]3−-doped 20.9 0.133 3.59 1.751As an additional functionality, we evaluated the anodicresponse of the POM-doped polymer films in the oxygen-evolution-reaction (OER) potential region. Measurementswere performed using a standard three-electrode setup inaqueous H2SO4 solution (pH 2). PBTTT films were drop-caston glassy carbon (GC) electrodes and doped with POM orbis(trifluoromethanesulfonyl)imide (TFSI−), a conventionalinert counteranion that can yield highly conducting PBTTTfilms.10) Current densities were normalized to the geometricarea of the GC electrode.Linear sweep voltammetry (LSV) curves show that[W6O19]2−-doped PBTTT exhibited a higher anodic currentdensity than [PW12O40]3−-doped and TFSI−-doped PBTTTin the OER potential region (Fig. 5(a)). This comparisonindicates that the enhanced anodic response is not simplyexplained by electronic conductivity. The [W6O19]2−-dopedelectrode also showed a smaller apparent Tafel slope than theTFSI−-doped and GC electrodes (Fig. 5(b)), suggesting morefavorable interfacial charge-transfer behavior.Controlled-potential electrolysis at 1.8 V vs. RHE fur-ther showed that the [W6O19]2−-doped PBTTT maintaineda higher current than the TFSI−-doped film over themeasurement period (Fig. 5(c)), suggesting a more sta-ble electrochemical interface under oxidative conditions.Electrochemical impedance spectroscopy (EIS) also showedthat the [W6O19]2−-doped PBTTT electrode had a lowercharge-transfer resistance (Rct = 345 Ω cm2) than the[PW12O40]3−-doped electrode (721 Ω cm2) (Fig. 5(d)). Thelarger impedance of the [PW12O40]3−-doped film is consis-tent with its greater structural disorder observed by GIWAXS,which may hinder interfacial charge transfer. Rct was sub-stantially larger than the high-frequency intercept of less than30 Ω cm2, which represents the combined series resistancearising from the electrolyte, electrode contacts, and elec-tronic conduction through the polymer film. This indicatesthat the impedance response under the present conditions isdominated by the interfacial charge-transfer process ratherthan by electronic transport through the polymer film. Theelectrochemically active surface area (ECSA) estimation isdescribed in the Supplementary Information (Fig. S4). Theestimated ECSA is consistent with only a limited, electrolyte-accessible region near the surface of the polymer film con-tributing directly to the electrochemical reaction. Thus, theobserved electrochemical functionality is governed primar-ily by dopant ions incorporated in the near-surface region,rather than by electrochemical processes occurring through-out the full film thickness, which would require diffusion ofwater and other reactant species into the hydrophobic filminterior. The enhanced anodic response is consistent with pre-vious studies of tungsten-oxide-based surfaces,35, 36) althoughW-based oxides and non-functionalized W/Mo/V POMsare not among the most active standalone water-oxidation081001-4© 2026 The Author(s). Published on behalf ofThe Japan Society of Applied Physics by IOP Publishing LtdAppl. Phys. Express 19, 081001 (2026) Y. Wang et al.Fig. 4. Hall measurements of a [W6O19]2−-doped PBTTT thin film. (a), (b) Hall voltage measured under magnetic fields at different temperatures.(c) Extracted carrier density and Hall mobility. (d) Temperature-dependent electrical conductivity.catalysts.37) Further exploration of POM structures and dop-ing processes may therefore enable systematic control ofboth transport and interfacial functionality in semicrystallinepolymer semiconductor films.We have demonstrated the incorporation of POMs intosemicrystalline PBTTT films by anion-exchange doping.[W6O19]2− was compatible with the PBTTT lamellar nanos-tructure and could be incorporated while preserving theordered film structure, yielding conducting organic–inorganichybrid semiconductor films with a conductivity of 200 Scm−1. Hall-effect and temperature-dependent conductivitymeasurements reveal partially coherent carrier transport coex-isting with hopping-like conduction in the divalent-anion-doped polymer semiconductor. The POM-doped films alsoshow an enhanced anodic response in the oxygen-evolutionpotential region compared with inert-anion-doped PBTTT,indicating interfacial electrochemical functionality beyondstable charge compensation. These results highlight POMdoping as a versatile strategy for functionalizing semicrys-talline polymer semiconductors with multivalent oxide-cluster ions. Because the charge, size, shape, and compositionof POMs are tunable, such tunability may open opportuni-ties to explore charge transport and interfacial electrochemicalfunctionality in semicrystalline thin films.081001-5© 2026 The Author(s). Published on behalf ofThe Japan Society of Applied Physics by IOP Publishing LtdAppl. Phys. Express 19, 081001 (2026) Y. Wang et al.Fig. 5. Electrochemical response of POM-doped PBTTT films in the oxygen-evolution potential region. (a) Linear sweeping voltammetry (LSV) at a scanrate of 10 mV s−1 and (b) Tafel plots of doped PBTTT and glassy carbon electrodes. 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