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. 2026 Oct 8. Online ahead of print. doi: 10.1039/d6sc06597j

Polymer-bridging energy transfer enables full-color erasable room-temperature phosphorescence with high stability in aqueous environments

Dongbo Chen a,b, Jiaxing Zhang a,b, Jiaxue Ren a,b, Jianzhong Fan c,✉, Jinzhu Ma b, Henggang Wang b, Zhenguang Wang a,b,✉, Andrey L Rogach d,✉
PMCID: PMC13670511  PMID: 42889958

Abstract

Achieving full-color, erasable, and stable photoactivated room-temperature phosphorescence (RTP) is often hindered by inefficient intersystem crossing, rapid triplet quenching and a low driving force for oxygen consumption, especially for deep-blue and red emissions. Herein, full-color photoactivated RTP materials, with ultralong emission lifetimes up to 4.18 s and reversibility over multiple write–erase cycles, are fabricated by doping organic phosphors into a polyvinyl butyral (PVB) polymer matrix. Unlike conventional inert hosts, PVB acts as an active energy transfer bridge that enhances host–guest energy transfer, promotes intersystem crossing and facilitates efficient oxygen consumption across a broad spectral range of 430–670 nm. The resulting films exhibit excellent stability in humid, acidic, alkaline, and saline environments, as well as full recyclability. Leveraging these properties, erasable photopatterning across multiple colors and scales, including large-area (20 × 20 cm) and fine-feature (2 mm) patterns, is demonstrated. Our results provide a general strategy to overcome key limitations in light-responsive RTP materials for dynamic anti-counterfeiting and rewritable data storage.

PVB acts as an active energy bridge in phosphor-doped films, enabling full-color photoactivated RTP with lifetimes up to 4.18 s, reversible write-erase, aqueous stability, recyclability, and erasable multicolor photopatterning.graphic file with name d6sc06597j-ga.webp

Introduction

Photopatterning, a non-contact methodology enabling spatial transfer of predefined patterns onto photosensitive material surfaces via controlled light irradiation, has become indispensable in anti-counterfeiting, information storage, bioengineering, and optoelectronics.1–3 Among its variants, erasable photopatterning has garnered particular interest due to its ability to repeatedly write and erase information, offering transformative potential for dynamic anti-counterfeiting and rewritable data storage.4–7 The realization of such reversibility critically depends on the intrinsic reversible photo-responsiveness of the constituent materials, which undergo controlled physical or chemical changes upon illumination and revert to their original state upon application of an external stimulus. Thus, the design of high-performance, reversibly photo-responsive materials represents a key strategic direction for advancing erasable photopatterning technologies.

Within this context, light-responsive room-temperature phosphorescence (RTP) materials have emerged as particularly promising candidates.8–10 They offer a combination of suitable optical attributes, including long-lived phosphorescence memory, large Stokes shifts, and high signal-to-noise ratios, and support reversible “write–erase” cycles triggered by external stimuli.11–13 To date, various photo-responsive RTP systems have been developed, including inorganic phosphors,14 liquid crystals,15 supramolecular assemblies,16 and carbon dots.17 However, these materials are predominantly limited to crystalline or amorphous powder forms and suffer from several inherent drawbacks such as poor mechanical flexibility, low processability, and limited film-forming capability. These constraints have motivated a shift towards polymer-based photo-responsive RTP materials, which offer superior processability, mechanical robustness, and biocompatibility.18–22

Conventional polymer-based RTP materials are typically fabricated by incorporating luminogens into a polymer host.23–27 In terms of erasable photopatterning, such composites exhibit oxygen-sensitive behavior, with freshly prepared films often showing negligible RTP due to quenching of triplet excitons by molecular oxygen (O2). Upon UV irradiation, O2 is consumed via energy transfer from triplet excitons of the guest molecules, leading to an increase in RTP emission. The phosphorescence then gradually fades as O2 rediffuses into the matrix. In this context, the polymer host primarily serves as a rigid scaffold that stabilizes triplet excitons and suppresses non-radiative decay (Fig. 1a). To enable reversible oxygen metabolism, the polymer matrix should possess sufficient free volume and chain mobility to permit O2 diffusion, which is an essential requirement for phosphorescence quenching and recovery. Ma and co-workers and Xin and colleagues doped organic phosphors into polyvinyl pyrrolidone (PVP) and polyvinyl alcohol (PVA) matrices, realizing UV-induced reversible RTP by balancing rigidity with moderate free volume of polymer matrices.28,29 However, O2 diffusion also facilitates the ingress of other external stimuli, particularly water vapor, leading to poor environmental stability of polymer matrices, especially under humid conditions or in aqueous media. To overcome this challenge, hydrophobic polymers have been engineered to shield guest molecules from water-induced quenching while still allowing efficient radiative transitions and O2 diffusion. Xu's group and Chen's group reported RTP systems based on epoxy matrices using molecular engineering strategies, significantly improving RTP performance under humid conditions.30,31 Nevertheless, these systems remained largely confined to cyan or green monochromatic emission, falling short of the requirements for multi-color displays and high-capacity information encoding. The fundamental limitation lies in the inefficient ISC of guest molecules and the poor stability of their triplet states. When targeting deep-blue emission, the major challenge is that high-lying triplet excitons are prone to non-radiative relaxation, leading to severe deactivation before light emission.32–37 In contrast, achieving red erasable RTP faces a different obstacle. The low-lying triplet energy level results in a diminished energy gap relative to ground-state molecular oxygen (3O2), thereby reducing the thermodynamic driving force for oxygen consumption, an essential process for erasable RTP photopatterning.19,38–40

Fig. 1. Schematic illustration of the design and application of full-color erasable RTP materials via a polymer-bridging energy transfer strategy. (a) Jablonski diagrams comparing the conventional polymer-stabilized approach (left) and the polymer-bridging energy transfer approach (right) for realization of photo-activated RTP films. (b) Design concept for full-color erasable RTP materials via host–guest doping. (c) Photographs of the composite films realized in this work under daylight (left) and 365 nm UV light irradiation (right). (d) Schematics of the working principle for erasable photopatterning applications using these full-color RTP films.

Fig. 1

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To address these challenges, in this study a polymer-bridging energy transfer strategy is proposed for producing full-color erasable RTP materials. Polyvinyl butyral (PVB) is not merely a rigid scaffold but serves as an active energy bridge that enhances host–guest energy transfer, promotes ISC across a broad spectral range, and facilitates efficient oxygen consumption (Fig. 1a). This strategy overcomes several intrinsic limitations of guest molecules, such as poor ISC efficiency, low triplet-state stability and oxygen consumption ability, enabling erasable afterglow from deep-blue to orange-red. Organic phosphors possessing programmable triplet-state dynamics are doped into the PVB matrix (Fig. 1b), producing full-color (from deep blue to red) photoactivated RTP materials with ultralong lifetimes up to 4.18 s and remarkable reversibility over multiple write–erase cycles. Leveraging PVB's excellent film-forming ability, large-area films are readily fabricated, with intense full-color RTP (Fig. 1c). Moreover, the hydrophobic–hydrophilic balance within PVB imparts exceptional water resistance without compromising reversible oxygen diffusion, thus supporting stable and erasable RTP in ambient and even harsh environments. Erasable photopatterning is demonstrated across multiple colors and film sizes (Fig. 1d), showing great potential in dynamic anti-counterfeiting and rewritable data storage.

Results and discussion

PVB is a random terpolymer derived from polyvinyl alcohol (PVA), comprising three monomeric constituents: polyvinyl butyral (PVBt), residual PVA, and polyvinyl acetate (PVAc).41–43 It was selected as a polymer host for three principal reasons: (i) its high glass transition temperature (from 70 to 84 °C) ensures a rigid environment at room temperature, effectively stabilizing triplet excitons; (ii) the PVA component provides abundant hydroxyl groups that establish a strong hydrogen-bonding network, further rigidifying the matrix, while the hydrophobic PVBt component imparts excellent water resistance, thereby protecting the hydrogen-bond network from moisture-induced disruption; and (iii) it exhibits a hydroxyl-rich rigid network and butyral-derived chain mobility, providing suitable energy levels that promote host–guest energy transfer.

Four guest molecules, namely dihydroindolo [2,3-a] carbazole (ICz), 9H-dibenzo[a,c] carbazole (DBCz), 5H-benzo[B]-carbazole (BCz), and 1-pyrenylboronic acid (PY) (Fig. S1), with programmable triplet-state dynamics were selected. Their electron-rich π-systems and nitrogen lone pairs enable hybrid (π, π/n, π) configurations that promote ISC. Heteroatom substitution further modulates spin–orbit coupling (SOC), whereas extension of π-conjugation enhances the (π, π*) character of the triplet state and reduces the singlet-triplet energy gap (ΔEST) (Table S1).44–46 In their dilute solutions, no delayed photoluminescence (PL) was observed at room temperature for all four molecules, due to dominant non-radiative relaxation. At 77 K, however, intense delayed PL, with emission maxima at 451 nm, 475 nm, 552 nm, and 600 nm, was observed for ICz, DBCz, BCz, and PY, respectively (Fig. S2).

To counteract thermal quenching, the four guest molecules were doped into PVB via drop-casting, yielding ICz@PVB, DBCz@PVB, BCz@PVB, and PY@PVB composites. Bare PVB films were also prepared as control samples. Leveraging PVB’s excellent film-forming ability, large-area films (>40 × 30 cm2) were readily fabricated (Fig. 1c). These films displayed high optical transparency (transmittance >60% in the visible region, with that for PY@PVB approaching 90%, as shown in Fig. S3) and outstanding flexibility (Fig. S4). Mechanical testing (Fig. S4 and Table S2) revealed a maximum tensile strength of 3.27 MPa and Young's modulus of 130.88 MPa for ICz@PVB, both exceeding the respective values of bare PVB.

Remarkably, all four films exhibited photoactivated RTP behaviors. In the pristine state, they showed only blue emission under 365 nm UV excitation, with no detectable afterglow. Upon photoactivation (365 nm, 30 mW cm−2) for 1 min, however, multicolored afterglow ranging from blue to orange-red, lasting up to 35 s, became clearly visible (Fig. 2a). Delayed PL spectra (Fig. 2b) showed broad emission maxima spanning from 430 to 670 nm, consistent with afterglow photographs and CIE coordinates (Fig. 2c) ranging from (0.15, 0.09) to (0.66, 0.34). The corresponding ultralong emission lifetimes of the four composite films ranged from 0.40 to 4.18 s (Fig. 2d). In addition, the irradiation-induced changes, excited at 275 nm and 450 nm, in delayed PL intensity are rather minor (Fig. S5). This indicates that the photoactivation in our system is highly wavelength-selective, which is likely related to the absorption characteristics of the photoactive moiety and the specific photochemical pathway required to populate the triplet emissive state. The films also show excellent stability against bending. Bending 100 times only resulted in a rather slight decrease (less than 5%) in the delayed PL intensity, with a negligible change in the average emission lifetime (2.68 s vs. 2.65 s), as shown in Fig. S6.

Fig. 2. Photophysical properties of full-color reversible RTP materials. (a) Photographs of four composite films before and after photoactivation, together with photographs taken after switching off the UV light for different time intervals. Prompt (dotted line) and delayed (solid line) PL spectra (b), CIE color coordinates (c), and emission decay curves (d) of the four composite films. Temperature dependent delayed PL spectra (e) and emission decay curves (f) of ICz@PVB. FTIR (g), Raman (h) spectra, and photocurrent curves (k) of bare PVB (cyan line), bare ICz (purple line), and ICz@PVB (blue line). (i) Energy level diagram of ICz@PVB. Evolution of the average emission lifetime of ICz@PVB recorded at 300 nm (l) and 380 nm (m), as a function of ICz doping concentration. (j) Energy level diagram of ICz and PVB with different molecular weights. (n) Prompt PL spectra of bare PVB (cyan line), UV-vis absorption spectra (dotted line, blue) and delayed PL excitation spectra (solid line, blue) of ICz@PVB. (o) PL excitation spectra of bare PVB (cyan line), and delayed PL excitation spectra of bare ICz (purple line) and ICz@PVB (blue line). (p) Simplified Jablonski diagram of the host–guest system, illustrating the difference between the conventional approach (left) and the polymer-bridging energy transfer strategy (right).

Fig. 2

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Temperature-dependent delayed PL measurements showed that as the temperature increased from 77 to 325 K, emission intensity gradually decreased and emission lifetimes shortened (Fig. 2e and f and Table S3), without peak shifting or spectral reshaping. These results are hallmarks of phosphorescence quenching via enhanced non-radiative decay.47,48 Notably, the peak shape and position matched perfectly with the 77 K delayed PL spectrum of pure ICz (Fig. 2e), confirming that the afterglow originated directly from the guest molecules. Analogous behavior was observed for DBCz@PVB, BCz@PVB, and PY@PVB (Fig. S7). In addition, no delayed PL signals were collected on the bare PVB film, without loading any guest (Fig. S8). Thus, the PVB matrix amplified the guest phosphorescence and imparted the photoactivation capability without altering the intrinsic emissive properties of the guests.

Structural and optical characterization studies were performed on ICz@PVB as a model system. XRD patterns (Fig. S9) showed two broad diffuse peaks at ∼21° and 29° for both bare PVB and ICz@PVB, confirming the amorphous nature of the films and the uniform dispersion of ICz without disrupting the polymer host structure. FTIR spectra (Fig. 2g) were nearly identical for bare PVB and ICz@PVB, except for some broadening of the O–H stretching band (3400–3500 cm−1) upon ICz incorporation, indicative of hydrogen bond formation.49 Raman spectroscopy (Fig. 2h) showed the retention of characteristic peaks of both PVB (2820, 3000 cm−1) and ICz (1314, 1649 cm−1), confirming successful encapsulation of ICz into the PVB matrix.50 XPS spectra (Fig. S10) revealed the expected C, O, and N signals, with high-resolution XPS spectra confirming the chemical integrity of ICz and the dominant role of hydrogen bonding in host–guest interactions. The high-resolution C 1s spectrum could be fitted with three peaks at 284.8 eV, 286.3 eV, and 287.5 eV, which were assigned to C–C/C Created by potrace 1.16, written by Peter Selinger 2001-2019 C, C–O, and C Created by potrace 1.16, written by Peter Selinger 2001-2019 N bonds, respectively (Fig. S10b).51 In the high-resolution O 1s spectrum of the ICz@PVB film, three peaks located at 531.4, 532.5, and 533.3 eV corresponded to C Created by potrace 1.16, written by Peter Selinger 2001-2019 O, C–O, and C–OH bonds (Fig. S10c). The high-resolution N 1s spectrum showed a single peak at 399.9 eV, attributed to the pyrrolic N of ICz (Fig. S10d).52

To rationalize the bright and ultralong afterglow observed for these composite films, time-dependent density functional theory (TD-DFT) calculations were performed, which predicted large ΔEST (0.96–1.45 eV) and small SOC constants (Fig. 2i and S11) for the guest molecules. These features typically preclude efficient ISC. Thus, we hypothesize that the polymer matrix acts not merely as a rigid scaffold but as an active energy bridge that assists the phosphorescence processes.

Given the computational complexity and analytical challenges associated with determination of the molecular orbital energy levels of the polymer, we employed its monomeric unit (n = 1), designated as PVB (n = 1), as a surrogate for theoretical investigation. The calculations revealed that PVB (n = 1) exhibits a higher highest occupied molecular orbital (HOMO) and a lower lowest unoccupied molecular orbital (LUMO) relative to the polymeric PVB. Furthermore, with increasing chain length (n value), a systematic elevation of the HOMO level and a concomitant depression of the LUMO level were observed (Fig. 2j and S12). Crucially, the LUMO of PVB was lower than those of the guests, and the HOMO of the guests was higher than that of PVB, rendering HOMO (guest)–LUMO (PVB) energy gaps sufficiently small to enable energy transfer.53 Photocurrent response measurements (Fig. 2k) showed increased current density upon higher guest loading, suggesting the presence of host–guest energy transfer. With the increase of the guest loading amount, an increase of emission lifetime at 300 nm (originated from PVB, Fig. 2l and Table S4) and negligible variation at 380 nm (originated from guest molecules, Fig. 2m and Table S5) were observed, confirming energy transfer from guest molecules to PVB. Significant spectral overlap between the prompt PL of bare PVB and the absorption/excitation spectra of the guests further supports this mechanism (Fig. 2n). Delayed PL excitation spectra showed two distinct bands corresponding to direct excitation of PVB and the guests, indicating transitions from both the polymer and guest singlet states to guest triplet states (Fig. 2o).

Collectively, these data support a photophysical mechanism in which PVB acts as an active energy bridge to facilitate the phosphorescence process. As shown in the simplified Jablonski diagram (Fig. 2p, left), in conventional systems, UV excitation populates the S1 state of the guest, followed by either fluorescence or the ISC process that results in phosphorescence. With the assistance of an energy bridge, the excited S1 state of the guest decays via fluorescence or energy transfer to the PVB matrix. The PVB polymer then facilitates ISC and transfers triplet excitons back to the guest T, dramatically enhancing phosphorescence efficiency and lifetime. This energy bridge effect rationalizes the apparent contradiction between DFT predictions and the experimental RTP performance, especially for the blue emissive guest molecules such as ICz that need to stabilize excitons in high-lying states. This PVB-mediated channel also explains why PVB participation offsets the intrinsic triplet-energy-driving-force limitation of red-emitting guests. For red guests such as PY, the low-lying T1 state provides only a small thermodynamic driving force for direct energy transfer from T1 to 3O2, so a guest-only oxygen-consumption mechanism would be inefficient. In our system, however, PVB is not a passive scaffold but an active energy bridge. It provides an additional O2-consumption pathway that is less dependent on the guest T1 energy, allowing O2 to be depleted efficiently even when the red guest’s intrinsic driving force is small. This is consistent with the experimental observation that ICz@PVB, DBCz@PVB, and BCz@PVB exhibit nearly identical photoactivation rates, while PY@PVB is only slightly slower. Thus, the PVB bridge shifts the competition toward oxygen depletion and enables reversible red/full-color RTP.

To elucidate the photoactivation process, we monitored delayed PL as a function of UV irradiation time (365 nm, 30 mW cm−2). For the four composites, the afterglow intensity increased with irradiation time, saturating after 30–80 s (Fig. 3a and S13). The effects of guest concentration on the delayed PL intensity of the composite film were studied. As shown in Fig. S14, the highest delayed PL intensity was observed upon loading 20 mg, 20 mg, 30 mg, and 20 mg of ICz, DBCz, BCz, and PY, respectively. Time-resolved measurements on ICz@PVB (Fig. 3b and Table S6) showed that the average emission lifetime increased from 4.24 µs to 2.50 s upon activation, reaching a maximum of 2.60 s. Further irradiation did not alter the lifetime. Similar trends were observed for DBCz@PVB (4.01 s), BCz@PVB (0.78 s), and PY@PVB (0.40 s) (Fig. S15 and Tables S7–S9). The RTP intensity enhancement factors were 393-fold, 9408-fold, 285-fold, and 2515-fold, respectively (Fig. 3c), with corresponding emission lifetime increases of 6.8 × 105-fold, 9.1 × 105-fold, 1.8 × 105-fold, and 7.7 × 104-fold, respectively (Fig. 3d).

Fig. 3. Photoactivated mechanism of full-color RTP materials. (a) Delayed PL spectra of ICz@PVB after varied photoactivation times ranging from 0 s to 40 s. (b) Delayed emission decay curves of ICz@PVB before and after photoactivation. The inset shows the delayed emission decay curves of the inactivated state. Comparison of the delayed PL intensity (c) and emission lifetimes (d) of ICz@PVB (i), DBCz@PVB (ii), BCz@PVB (iii), and PY@PVB (iv) before (red) and after (blue) photoactivation. (e) Delayed PL spectra of ICz@PVB after photoactivation and varied deactivation times ranging from 0 s to 90 min. (f) Afterglow images (top) and corresponding delayed PL lifetime variations (bottom) of ICz@PVB during activation–quenching cycles. (g) FTIR spectra of ICz@PVB before and after photoactivation at 30 s and 60 s. Delayed PL spectra (h) and emission decay curves (i) of ICz@PVB measured in air and under vacuum. (j) EPR spectra of ICz@PVB using TEMP as a spin-trapping agent before and after photoactivation at 5 min and 10 min. (k) Calculated ISC rate constants (kISC) of four bare guest molecules: kISC (S1–T1) (solid bars) and kISC (S1–T2) (shaded bars). (l) Energy level diagram of four bare guest molecules and molecular oxygen, illustrating the relative positions of the T1 states and the triplet ground state (3O2) and singlet excited states 1O2 (1Δg, 0.98 eV; 1Σg+, 1.63 eV). (m) Normalized delayed PL intensities of ICz@PVB, DBCz@PVB, BCz@PVB, and PY@PVB films as a function of photoactivation time. (n) UV-vis absorption spectra of PVB films doped with ABDA under 365 nm UV irradiation for different irradiation times. (o) Proposed mechanism of full-color photoactivated RTP, based on a PVB-mediated oxygen consumption process.

Fig. 3

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Notably, increasing the excitation power from 30 to 365 mW cm−2 significantly shortened the activation time (Fig. S16 and S17), which can be attributed to accelerated O2 consumption under high power irradiation. Under high-power UV irradiation (365 mW cm−2), the delayed PL intensities of the four composite films, loaded with different guest molecules, reached their maximum values within 10 s (Fig. S12a–d). In contrast, when irradiated at a lower power of 30 mW cm−2, the same process required as long as 40 s. A similar dependence was observed in the evolution of delayed emission time as a function of photoactivation duration (Fig. S13a–d). Higher excitation power also improved the final phosphorescence performance, as a more oxygen-depleted environment suppressed non-radiative decay. Remarkably, the photoactivation process was fully reversible: activated films returned to their initial state within 90 min under dark ambient conditions (Fig. 3e and S18). Heating at 60 °C accelerated the recovery speed (Fig. S19), so that the films returned to their initial state in 10 min. This “activation–quenching” cycle remained stable over at least 10 repeats with a negligible loss in afterglow performance (Fig. 3f), establishing a robust foundation for erasable photopatterning.

Mechanistic insights were further gained through FTIR, UV-Vis, EPR, and controlled atmosphere experiments. Upon UV irradiation (365 nm, 30 mW cm−2, for 60 s), FTIR spectra showed broadening and decreased intensity of the O–H band (∼3450 cm−1) and diminished C Created by potrace 1.16, written by Peter Selinger 2001-2019 O (1733 cm−1) and C Created by potrace 1.16, written by Peter Selinger 2001-2019 C (∼1630 cm−1) peaks, indicative of photo-crosslinking (Fig. 3g).54 UV-vis absorption decreased at 250–270 nm and 326 nm, further confirming the occurrence of photo-crosslinking (Fig. S20).55 Compared to measurements taken in air, the films tested under vacuum exhibited intense afterglow, with a 208-fold increase in delayed photoluminescence intensity (Fig. 3h) and a pronounced extension of emission lifetime from 4.24 µs to 1.65 s (Fig. 3i). Notably, these effects occurred without any pre-activation and could not be reversed by heating, confirming that ambient oxygen is the primary quencher of the emission.

Electron paramagnetic resonance (EPR) spectroscopy revealed no signal before UV irradiation, but a distinct signal with g ≈ 2.0030 (characteristic of a free electron) emerged upon UV exposure, with its intensity increasing with irradiation time (Fig. S21).56 Using 2,2,6,6-tetramethyl-4-piperidone hydrochloride (TEMP) as a spin trap, we detected a strong signal corresponding to singlet oxygen (1O2) after photoactivation (Fig. 3j). These results demonstrate that UV irradiation drives conversion from 3O2 to 1O2, effectively removing molecular oxygen and suppressing the quenching of triplet excitons. Subsequent natural or thermally accelerated re-diffusion of 3O2 into the film erases the afterglow.

To gain deeper insight into the oxygen consumption process, the speeds of photoactivation and recovery of the films doped with different guest molecules were investigated. Theoretically, the photoactivation speed is related to the oxygen consumption rate of the guest molecule, which is determined by the KISC value of the guest molecules and the driving force for the energy transfer to 3O2.56 As shown in Fig. 3k and Table S10, KISC values exhibited substantial differences, ranging from 1.10 × 10−5 to 9.78 × 103 s−1 across the four guest molecules. In addition, the driving forces for energy transfer from the triplet state of the guest molecules to 3O2 also showed obvious differences, following the order ICz > DBCz > BCz > PY (Fig. 3l). However, these theoretical simulation results contradicted the experimentally determined photoactivation and recovery rates derived from the delayed PL spectra measurements. The photoactivation speed was further evaluated by analyzing normalized delayed PL intensities of composite films as a function of photoactivation time. A linear regression was conducted using the data from the start to the end of the transition. The slope of the fit quantifies the rate of photoactivation, denoted as k. As illustrated in Fig. 3m and Table S11, the photoactivation speed followed the order ICz (k1 = 0.11) = DBCz (k2 = 0.11) = BCz (k3 = 0.11) > PY (k4 = 0.09), while the four films exhibited nearly identical recovery behaviors (Fig. S22). This contradiction can be attributed to the involvement of PVB in the oxygen consumption process, wherein the excited electrons in PVB are transferred to 3O2. This hypothesis was confirmed by collecting the UV-visible absorption spectra of 9,10-anthracenediyl-bis (methylene) dimalonic acid (ABDA) (Fig. 3n), a sensitive singlet oxygen indicator. UV irradiation treatment of PVB + ABDA resulted in a decrease in optical density, while only a slight variation of absorption intensity (less than 10%) was observed in the case of pure ABDA (Fig. S23). This confirms that the singlet oxygen generation is PVB-mediated. In addition, similar spectrum behaviours were observed in the absence and presence of ICz (Fig. S24), suggesting that there is no interference with the singlet oxygen generation ability after loading guest molecules.

Based on the above results, we propose a PVB-bridging oxygen consumption mechanism for achieving full-color (deep blue to red) photoactivated RTP. In the conventional oxygen consumption process, energy transfer occurs directly from the triplet state of guest molecules to 3O2 (Fig. 3o, left panel). Under this mechanism, deep blue and red emissions are difficult to realize due to the relatively low stability of electrons in high-lying triplet states and the low KISC rates or small driving forces. With the assistance of the PVB bridge, the polymer matrix facilitates indirect energy transfer or electron mediation between the guest triplet states and molecular oxygen, so that the constraints imposed by the guest's intrinsic triplet properties are alleviated. Consequently, the PVB-bridging pathway enables efficient oxygen consumption and robust photoactivation across a broad spectral range, reconciling the observed experimental results with the proposed mechanism.

Crucially, the hydrophobic PVBt component of PVB confers exceptional stability on the produced composites in humid and aqueous environments. After immersion in water, HCl (pH = 1), NaOH (pH = 13), or saturated NaCl for 40 days, ICz@PVB showed no emission quenching and retained a long-lived afterglow visible to the naked eye for 15 s (Fig. 4a and b). Emission lifetimes remained nearly constant (Fig. 4c and d) after immersion for 40 days. This outstanding environmental robustness is a key advantage over prior RTP systems. Furthermore, the films were fully recyclable due to their dynamically reversible non-covalent cross-linking network. Fragments of ICz@PVB could be redissolved and recast into intact films (Fig. 4e). Even after five recycling cycles, the afterglow performance remained excellent, with emission intensity retaining 89–98% of the initial value (Fig. 4f). A slight decrease was observed in the emission lifetime (Fig. 4g), caused by the changes in the polymer density of films, after the recycle process. This recyclability significantly reduces environmental waste and enhances practical applicability of these composite films.

Fig. 4. Stability and recyclability of composite films. (a and b) Afterglow images of ICz@PVB films after immersion in different solvents for 0 and 40 days, respectively. (c and d) Evolution of delayed emission lifetime of ICz@PVB films as a function of immersion time in different solvents, including pure water (blue, solid bars), aqueous solution of NaCl (blue, shaded bars), HCl (purple, solid bars), and NaOH (purple, shaded bars). (e) Recycling process of ICz@PVB films and afterglow images taken after five consecutive recycling cycles. Delayed PL spectra (f) and emission lifetimes (g) of ICz@PVB films during five recycling cycles.

Fig. 4

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Leveraging the exceptional optical and mechanical properties of the composite films realized in this study, we further explored information storage and rewritable patterning. Produced by a mask photo-printing method on an 8 × 8 cm DBCz@PVB film, a complex pattern remained clearly visible for 5 min and completely faded in a natural disappearance process after 20 min (Fig. 5a), demonstrating the potential for temporary information storage. Large-area (20 × 20 cm) DBCz@PVB films enabled photo-printing of fine patterns (feature sizes as small as 2 mm) via patterned masks (Fig. 5b). After 1 min of activation (365 nm, 365 mW cm−2), those patterns remained well preserved and became naturally erased within 20 min under ambient conditions. Four sequential write–erase cycles of different patterns were successfully demonstrated. To highlight the universality of this approach, we prepared films with three distinct afterglow colors (blue, red, and yellow) and achieved optical printing and reversible cycling across different sizes (from 2 × 2 cm to 8 × 8 cm) and colors (Fig. 5c–e). Notably, on a yellow afterglow BCz@PVB film, three different Chinese characters (“红”, “荷”, and “花”) were sequentially written and erased (Fig. 5e), underscoring the high information capacity and versatility. Collectively, these results establish that PVB-based RTP composite films are a powerful platform for erasable photopatterning across multiple colors, scales, and environmental conditions.

Fig. 5. Erasable photopatterning. (a) Time-dependent natural disappearance process of patterns printed on DBCz@PVB films via a mask photo-printing method. (b) Schematic illustration of rewritable photopatterning on DBCz@PVB films, where erasure occurs via natural time-dependent quenching. (c–e) Photopatterning and cycling processes of ICz@PVB (c), BCz@PVB (d), and PY@PVB (e) films, where pattern erasure is driven by thermally induced quenching.

Fig. 5

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Experimental section

Materials

Polyvinyl butyral (PVB) and 9,10-anthracenediyl-bis (methylene) dimalonic acid (ABDA) were provided by Innochem. 11,12-Dihydroindolo[2,3-a] carbazole (ICz) and 1-pyrenylboronic acid (PY) were provided by Aladdin. 9H-Dibenzo[a,c]carbazole (DBCz) was provided by Adamas. 5H-Benzo[B]-carbazole (BCz) was provided by Macklin.

Characterization

The prompt and delayed photoluminescence (PL) spectra of the materials were recorded on a Hitachi F-7000 spectrofluorometer. The temperature-dependent prompt and delayed PL spectra and time-resolved decay curves were measured on a Horiba Fluoromax+ spectrofluorometer. The emission lifetimes were measured on an FS5 spectrofluorometer (Edinburgh). X-ray diffraction (XRD) patterns were collected at room temperature on a Bruker D8 Advance diffractometer (Cu Kα radiation, λ = 1.5418 Å). X-ray photoelectron spectroscopy (XPS) was performed on a Thermo Scientific Escalab 250Xi+. Fourier-transform infrared (FTIR) spectra were acquired on a Thermo Scientific Nicolet iS10 spectrometer. Electron paramagnetic resonance (EPR) spectra were measured on a Bruker A300. UV-visible and transmittance spectra of films were measured on a Hitachi U-3900 UV-Vis spectrophotometer. Static tensile tests were conducted using a Shimadzu AGS-X instrument at a tensile rate of 2 mm min−1. Photocurrent measurements were performed on a CH Instruments electrochemical workstation equipped with a PerfectLight PLS-SXE300+ xenon lamp as the excitation source. The ICz, PVB and ICz@PVB films coated on indium tin oxide (ITO) conductive glass served as working electrodes, which were immersed in 0.2 M Na2SO4 aqueous electrolyte. Glassy carbon and Ag/AgCl were used as counter and reference electrodes, respectively. The photocurrent curves were collected without external bias.

Theoretical calculation

Geometry optimizations of the ground state (S0) and excited states (S1, T1, and T2) were performed using the PBE0 functional with the 6-31G* basis set. The adiabatic energy gaps between the relevant excited states were further used to determine ΔE(S1–T1) and ΔE(S1–T2). On this basis, spin–orbit coupling (SOC) matrix elements between S1 and T1 as well as between S1 and T2 were computed using the ORCA program package. Subsequently, the intersystem crossing (ISC) rate constants (kISC) for the S1 → T1 and S1 → T2 channels were evaluated using the MOMAP program.

Preparation of the bare PVB film

2.0 g of PVB was dissolved in 20 mL methanol and transferred into a 50 mL beaker. The mixture was magnetically stirred at room temperature for 1 h and then ultrasonicated for 30 min to obtain a viscous transparent solution. After standing for 1 h, the solution was cast onto a clean glass substrate and dried in an oven at 45 °C for 12 h to remove the solvent, giving the target PVB film.

Preparation of afterglow materials

Herein, preparation of 1.0 wt% ICz@PVB is described as an example. 20 mg of ICz was dissolved in 20 mL of methanol and transferred into a 50 mL beaker, followed by addition of 2 g of PVB powder. The mixture was magnetically stirred at room temperature for 1 h, followed by ultrasonication for 30 min to ensure complete dissolution. After standing for 1 h, the solution was cast onto a clean glass substrate and dried in an oven at 45 °C for 12 h to remove the solvent, yielding the target ICz@PVB film. The fabrication process for other guest molecule films was the same as above.

Conclusions

In summary, a set of full-color, photoactivated RTP materials was produced by doping organic phosphors into a PVB polymer matrix. PVB serves as an active energy bridge that promotes host–guest energy transfer, stabilizes triplet excitons, and enhances ISC and oxygen consumption efficiency across a broad spectral range of 430–670 nm, thus enabling efficient and reversible oxygen-mediated phosphorescence activation. This mechanism effectively circumvents the intrinsic limitations of guest molecules, thereby achieving deep-blue to orange-red reversible afterglow in a single polymer platform. The resulting films exhibit outstanding mechanical flexibility, environmental robustness (stable for 40 days in water, acid, base, and saline), and full recyclability. Erasable photopatterning is demonstrated across multiple colors, film sizes and complex patterns, including fine features down to 2 mm and sequential multi-character writing. These results provide a general strategy to overcome key limitations in light-responsive RTP materials and open new avenues for their practical photopatterning applications.

Author contributions

D. Chen and Z. Wang conceived the project. D. Chen designed and performed the main experiments, analyzed the data, and wrote the original draft. J. Zhang and J. Ren contributed to part of experiments. J. Fan performed the TD-DFT calculations, analyzed the results, and revised the manuscript. J. Ma and H. Wang contributed to material characterization, and data analysis. Z. Wang supervised the project, acquired funding, and revised the manuscript. A. L. Rogach supervised the work, provided resources, and revised the manuscript. All authors discussed the results and approved the final manuscript.

Conflicts of interest

There are no conflicts to declare.

Supplementary Material

SC-OLF-D6SC06597J-s001

Acknowledgments

This work was financially supported by the National Natural Science Foundation of China (Grant 22175052), the Natural Science Foundation of Hebei Province (Grant B2025205014), the Hebei Province Higher Education Scientific Research Project (JCZX2025005), the Hebei Normal University Science and Technology Fund Project (L2025B16 and L2026B11), and the Centre for Functional Photonics of City University of Hong Kong.

Data availability

All the data are available on request from the authors.

Supplementary information (SI) is available. See DOI: https://doi.org/10.1039/d6sc06597j.

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Associated Data

This section collects any data citations, data availability statements, or supplementary materials included in this article.

Supplementary Materials

SC-OLF-D6SC06597J-s001
SC-OLF-D6SC06597J-s001.pdf (3.1MB, pdf)

Data Availability Statement

All the data are available on request from the authors.

Supplementary information (SI) is available. See DOI: https://doi.org/10.1039/d6sc06597j.

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