Jagriti Ahujaa,
Saurabh Pandeya,
Shital Devinderb,
Jyoti Sardanaa,
Anupriya Tiwaria,
Nagarajan Subramaniyamc and
Joby Joseph*ade
aPhotonics Research Lab, Physics Department, Indian Institute of Technology, Delhi, New Delhi, Delhi 110016, India. E-mail: joby@iitd.ac.in
bCentre for Sensors, Instrumentation, and Cyber Physical System Engineering, Indian Institute of Technology Delhi, New Delhi, Delhi, India
cX-Fold Imaging oy, FL-00076 Espoo, Finland
dOptics and Photonics Centre, Indian Institute of Technology Delhi, New Delhi, Delhi 110016, India
eIndian Institute of Technology Delhi – Abu, Dhabi, Zayed City, Abu Dhabi, United Arab Emirates
First published on 30th July 2025
Utilizing fluorescent emitters with precisely designed nanostructures regulates their emission characteristics, which has great potential in light-emitting devices, biosensing, and quantum technologies. In this context, we propose a large area nanostructured design on a flexible polyethylene terephthalate (PET) substrate by patterning it in a square periodic symmetry and coating it with a TiO2 thin layer to demonstrate cost-effective photoluminescence enhancement and directionality. The proposed design enables a controlled light emission enhancement of about 110 times from the emitter layer over the array through resonance-mediated light confinement. Such mode confinement leads to an increase in the local density of states, which leads to a 100-fold increase in the Purcell factor. Beyond amplification, the polarization-dependent excitation of GMR modes enables directional coupling of photoluminescence into the radiative zeroth-order channel, resulting in well-defined angular emission profiles, as validated by angle-resolved spectroscopy and back focal plane imaging for both transverse electric and transverse magnetic polarization of incident light. The proposed large-area photonic array on a PET substrate offers potential for incorporation into advanced light-emitting optical devices, owing to its scalability and adaptability for practical applications.
Integrating photonic nanostructures with emitter layers has significantly improved light emission control, enhancing both PL intensity and directionality.9,10 Various periodic nanostructures, including plasmonic11–13 and dielectric configurations,14–17 have been explored to tailor emission properties. Plasmonic nanostructures leverage plasmon resonance to enhance light–matter interactions; however, they suffer from intrinsic ohmic losses18 and PL quenching due to nonradiative energy transfer to metals,19 limiting their efficiency. In contrast, dielectric periodic nanostructures, such as photonic crystals, topologically engineered platforms20,21 and metasurfaces, enable efficient light confinement, high-quality factor, and coupling without these losses.22,23 The periodic arrangement of nanostructures leads to resonant nanophotonic effects mediated by diffraction effects such as Rayleigh anomalies and surface lattice resonance. The close proximity of the waveguide layer to such a lattice arrangement leads to a diffraction-coupled waveguide mode, known as guided-mode resonance (GMR).24 Guided-mode resonance (GMR) in dielectric nanostructures integrated with a waveguide layer provides robust PL directional amplification25 by modifying the local density of states (LDOS) of emitters26,27 and by redistributing the emitted light into specific angles with minimal loss, outperforming other periodic structures.
Recent studies utilizing periodic structures have shown varying degrees of PL enhancement (N-fold) with controlled light emission via resonant light–matter interactions. Rigid dielectric metasurfaces and photonic crystal cavities have shown high PL enhancement factors by leveraging high-Q Fano resonances (1000 fold),28 cavity mode resonance (2400 fold),29 surface lattice resonance,30 symmetry breaking and spin–momentum locking (45 fold)20,21 or through collective Mie resonances (10 fold),31 but these require complex fabrication techniques such as e-beam lithography and semiconductor epitaxy, lack mechanical flexibility with limited scalability and exhibit limited Purcell effects with no angular control. However, for practical applications, it is crucial to fabricate these photonic nanostructures over large areas such as light-emitting diodes (LEDs),32 single-photon sources,33,34 lasers6,25,35,36 and bio-imaging systems,37,38 ensuring uniform enhancement across the entire emission region, while maintaining the mechanical flexibility to ensure scalability and integration into real-world devices.
In this work, we present the design and study of a dielectric photonic array composed of patterned flexible polyethylene terephthalate (PET) in a square lattice with a TiO2 thin layer coated over it. The fabrication is carried out through the nanoimprint lithography process, resulting in a large area periodic structure. This configuration integrates the flexibility and cost-effectiveness of PET with the high refractive index of TiO2, functioning as a foundational element for improved light–matter interaction. When irradiated with transverse electric (TE)/transverse magnetic (TM) polarized light with respect to the sample, the nanostructure supports the corresponding GMR modes in the visible spectrum. A comprehensive insight into the origin of these modes has been elaborated to highlight their impact on the LDOS, which prominently plays a vital role in PL enhancement via the Purcell effect. The optical dispersion curves obtained experimentally and the associated mode analyses are corroborated by simulation findings utilizing the Lumerical finite-difference time-domain (FDTD) solver39 and with analytical calculations.
Furthermore, we leveraged the strong local field confinement in the dielectric array to demonstrate the phenomenon of enhanced light emission by coating a thin layer of the fluorescent dye Coumarin 481. The enhancement mechanism is attributed to the strong interaction between the PL emission from the dye layer and the diffraction-related photonic modes supported by the structure. The presence of these resonance modes in the structure not only shows an enhancement of 110 times in the emitted light but also spatially redistributes the earlier broad PL emission from the dye into well-defined angles in specific angular directions.40 Additionally, by collecting the emitted light at different angles, we establish a direct correlation between the optical extinction spectra and the PL dispersion curves for TE and TM polarization of incident light, further providing validation for the interaction between the GMR modes and the emitted fluorescence. Furthermore, back focal plane (BFP) imaging provides direct visualization of these spatially controlled emission patterns from the dielectric array. The insights gained from this work would significantly enhance tunable light emission applications for next-generation optical devices, including large area light-emitting diodes, polarization-sensitive biosensors, advanced spectroscopic tools, directional emitters, and fluorescence-based bioimaging.
The array's configuration shape is meticulously designed to ensure that the GMR under normal incidence aligns with the primary emission peak of the Coumarin dye at around 500 nm. The square periodic PET nanopillar, as shown in the scanning electron microscopy (SEM) image in Fig. 2(a), possesses a height (H) of 30 nm and a radius (R) of 85 nm, situated within a square lattice characterized by a periodicity (P) of 300 nm along the x and y axes (fill factor ff = 67.11%), validated by atomic force microscopy (AFM) (Fig. 2b). For the analysis, the plane of incidence (POI) is set to be in the x–z plane, such that the incident wave vector (k) resides in this plane. When the polarization of the electric field vector (E) is oriented orthogonal to the POI, i.e., along the y-axis, this configuration corresponds to TE polarization. In contrast, when E is located within the POI, it corresponds to TM polarization. A solution of C481 dye with a concentration of 1 mM in ethanol was mixed with an aqueous PVA solution (0.25 wt%) in equal parts. This mixture was spin-coated onto a nanostructured sample substrate at a speed of 1500 rpm for 30 seconds, resulting in a film thickness of 300 nm (section S2). The coated sample was then heated at 95 °C for 2 minutes to evaporate the solvents. The PVA–dye solution shows an absorption peak at 400 nm, while the thin film exhibits a fluorescence peak at 500 nm, with a full width at half maximum (FWHM) of 80 nm, as illustrated in Fig. S2 of the ESI.†
To ensure the reliability of the emission data, all the measurements were performed on the ensembles of dye molecules, which effectively average out transient blinking events. Each PL measurement was acquired rapidly, with minimal exposure time for each sample to minimize the impact of photobleaching. Additional excitation power-dependent and photostability measurements on the dye-coated PET–TiO2 array were also conducted and are provided in section S3 of the ESI.†
![]() | (1) |
![]() | (2) |
The relationship (1) for the normal angle of incidence (θi = 0) is further reduced to eqn (3) for the periodicity ‘a’, providing the effective refractive index satisfied by the diffracted orders in the waveguide media.13
![]() | (3) |
The effective index of the diffracted orders is calculated and plotted along with the effective index of the TM and TE waveguide modes supported by the designed photonic array, as shown in Fig. 3(b). A waveguide mode solver was used to evaluate the effective index of the waveguide modes44 supported by the photonic array. Whenever the effective index of the diffracted order equals the effective index of the waveguide mode, it excites a GMR mode. It can further be inferred that the mode at 515 nm corresponds to the TE waveguide mode, while the mode at 491 nm is attributed to the TM waveguide mode45 for TM polarization of input light. To further confirm the nature of the modes, the electric field distributions of each GMR mode corresponding to their respective resonant wavelengths along the XZ, XY, and YZ cross-sections are plotted in Fig. 4. The peak at 491 nm corresponds to propagation along the X-axis ( is parallel to
(grating vector), TM mode), whereas for 515 nm, propagation along the Y-axis results in the TE mode (
is perpendicular to
). Furthermore, the polarization degeneracy of GMR under normal illumination is due to the cylindrical symmetry and square periodicity of the photonic array.46 Detailed analysis of these modes, calculated using electromagnetic mode treatment of a slab waveguide, is presented in sections S5–S7 of the ESI.† Fig. 3(c) and (d) present the experimentally obtained optical extinction spectra of the photonic array as a function of the incident angle (θin) for both TE and TM polarized incident light, respectively. The simulated extinction spectra exhibit strong concordance with the observed extinction spectra (Fig. 3(e) and (f)). A translucent dashed square box in the dispersion curve indicates the dye emission band. As denoted in Fig. 3(c and e) for TM polarization, the (±1, 0) order shows a non-degenerate nature, i.e., they split into two branches at oblique incidence, and is associated with the TM-GMR (491 nm, propagation along the X-axis), while the (0, ±1) order is degenerate in nature, showing a nearly flat dispersion curve with no splitting at oblique incidence and is associated with the TE-GMR (515 nm, propagation along the Y-axis). In contrast, the reverse occurs for the TE polarization excitation as anticipated. In TM waveguide modes, the electric field vector under normal TM excitation (P-polarization) lies parallel to the plane of incidence (x–z plane)47 and propagates along the x–z plane, producing a resonance at 491 nm. To gain more insight into the TM-GMR mode, we have plotted the simulated |E|2 for a resonance wavelength of 491 nm in the x–y, y–z, and x–z planes (Fig. 4a). The high refractive index contrast between the TiO2 layer and the surrounding medium results in a substantial near-electric field enhancement (|E|2 > 40) at the top edges of the TiO2–PET nanostructures, which in turn facilitates mode propagation along the x direction. TE waveguide modes, on the other hand, show distinct behaviour. The electric field vector is directed orthogonally to the direction of propagation, in the y–z plane.45 Fig. 4b shows the electric field confinement for TE-GMR mode in the x–y, y–z, and x–z planes, revealing the mode confinement along the y direction. It ensures that the electric field is localized within the structure, which is crucial for fluorescence enhancement in the presence of an emitting dye.
![]() | ||
Fig. 4 Electric field distribution with TM polarization of incident light: (a) λTM-GMR = 491 nm and (b) λTE-GMR = 515 nm in (i) x–y, (ii) y–z and (iii) x–z directions, respectively. |
The improvement of photoluminescence in the nanostructured array is determined collectively by extended light–emitter interaction, modifications in radiative decay rates, and efficient light extraction.10 Excitation of GMR aligned with the emission wavelength of the emitter results in near-field coupling of confined electromagnetic field density. This boost in the interaction supports the increased local density of states (LDOS) with an improved radiative recombination rate. This is based on Fermi's “golden rule”, where the spontaneous emission rate of an emitter in the weak coupling regime can be modified by tailoring the LDOS.48 Consequently, the presence of nanostructures modifies the LDOS of the emitters by providing new decaying channels in their near field, which directly affects the decay rate of the emitters.49 The spontaneous emission decay rate is measured as50
![]() | (4) |
The Purcell factor enhancement is one of the crucial parameters in quantifying the modification in the emission decay rate,52 which is the ratio of the LDOS in the presence of nanostructures to the free space LDOS. The Purcell factor is expressed as:52,53
![]() | (5) |
The Purcell factor is often approximated using the formula
![]() | (6) |
![]() | (7) |
As shown in Fig. 5a, an enhancement in the LDOS of approximately 100 at a wavelength of 515 nm was observed for emitters placed at the top nanocylinders, indicating a sharp increase in the density of states in comparison with the free space. This peak aligns with the TE-GMR condition at λ = 515 nm of the photonic array. This increase of the LDOS, as indicated by eqn (5), is precisely proportional to the ratio of the radiative decay rate and gives a Purcell Factor enhancement of 100. The analytically derived decay rate curve, obtained using eqn (4), shows a notable increase the TE-GMR wavelength for the photonic array relative to the background decay in air, demonstrating effective emitter-mode coupling and increased spontaneous emission, as shown in Fig. 5b. The spatial and orientational dependence of the relative LODS for the emitter is further discussed in section S8 of the ESI.† Both the relative LDOS and the spontaneous decay rate curve show a relatively smaller peak, λ = 495 nm, corresponding to the TM-GMR condition. This reduced LDOS is attributed to its lower Q factor and broader spectral width compared to the TE-GMR mode. This indicates that the observed increase in emission from the emitter layer is attained through the utilization of the waveguide modes facilitated by the photonic array. For completeness, the Purcell factor is also calculated using eqn (6) through FDTD simulation, and the results are discussed in section S9.
To further support the calculated LDOS enhancement, time-resolved photoluminescence (TRPL) measurements were performed, which reveal a significant drop in the average dye PL lifetime from 3.37 ns on the reference substrate to 0.15 ns when coupled to the photonic array at the GMR wavelength (515 nm). This substantial reduction in lifetime gives direct experimental proof of the Purcell factor enhancement, confirming that the enhanced LDOS indeed leads to a higher spontaneous emission rate. The detailed decay fitting and analysis are provided in section S10 of the ESI.†
The interaction of PL emission with GMR is further confirmed by examining angle-resolved photoluminescence spectra for TE- and TM-polarized excitation (λ = 405 nm), as shown in Fig. 6(b and c), where the sample was excited normally and emission was recorded as a function of θem. The momentum-space behavior of the emission spectra is consistent with the angular GMR extinction dispersion observed, as shown in Fig. 3(c and d). This directly supports the excitation of waveguide leaky mode by the emission wavelengths of the emitter, which corresponds to various k vectors of the emitted light, ultimately leaking and coupling with zeroth-order diffracted light. The PL amplification takes place precisely at wavelengths that align with the extinction peaks observed in the dispersion curves, with no anti-crossing or Rabi splitting behavior, showing the absence of strong coupling.58,59 Furthermore, the dye emission exhibits a relatively broad spectral bandwidth (∼80 nm), which exceeds the resonance splitting required to resolve vacuum Rabi modes.60,61 This suggests that the emission is notably influenced by the resonant excitation of moderate Q-factor of GMR modes, thereby affirming that the robust near-field coupling between the emitters and the waveguide modes is via the Purcell effect (weak coupling regime) and plays a pivotal role in engineering the directionality of light emission.
Furthermore, we recorded the back focal plane images of the PL emission pattern to validate its directional amplification abilities, where the emission pattern was recorded in the momentum space from the photonic array consisting of the emitter layer. These images contain information about the intensity of emitted light in different directions in the Fourier plane. BFP images were recorded using a home-built setup (Fig. 7a) with a collimated 405 nm continuous wave laser as the excitation source. The PL emission from the sample is collected using a Nikon Plan Fluor 40× objective with 0.75 numerical aperture (NA) and directed toward a CCD camera after propagating through a dedicated 4f lens system and a 425 nm long pass filter. The PL intensity distribution in momentum space, PL(kx,ky), is represented by the back-focal plane of the collection objective, which is imaged using the CCD camera. This distribution is then transformed into the angular distribution, PL(θ,ϕ), using the following coordinates:62,63
PL(ky,ky) = PL(θ,ϕ)(cosθ)−1 | (8) |
ky = k0![]() ![]() | (9) |
kx = k0![]() ![]() | (10) |
where k0 is the wave vector in free space and θ and ϕ represent the zenith and azimuth angles (which signify the k vector angle with the normal z direction and its projection angle in the xy plane) in spherical coordinates, respectively. The maximum angle θem for collecting the photoluminescence is constrained by the NA of the collection objective employed in the experiment, i.e., 0.75. A polarizer was employed in the detection path to differentiate various components of the emission. The far-field emission from the reference sample is utilized to compare with the emission pattern derived from the photonic array. The BFP image of the unpolarized PL from the dye-coated photonic array is shown in Fig. 7c. The white dotted circles indicate the greatest angle (θem = 48.5 degrees) that can be captured using an objective with a numerical aperture (NA) of 0.75 from the sample normal. The BFP image exhibits a 4-fold symmetry because of the diffraction from a square periodic lattice and is normalized to its maximal value to facilitate comparative analysis. It is observed that the bands of high emission intensity in the BFP image are superimposed on the background emission originating from dye molecules that remain uncoupled to any resonant mode supported by the structure. The difference in the emission pattern compared to the reference sample indicates strong near-field coupling between the waveguide GMR modes and the light emitted by the emitters. The periodicity of the photonic array imposes momentum-matching conditions that selectively enhance certain propagation directions, effectively redistributing the emitted photons along those directions. The interaction of localized emitter dipoles with the structured optical modes of the array generates this directional control by means of constructive and destructive interference, leading to modified radiation patterns of the dye emitters. Furthermore, we also analyzed BFP images of the emission for TE and TM polarization states to examine the polarization filtering response in the emission pattern. Fig. 7d and e illustrate the emission patterns obtained with a polarizer positioned just before the camera with its pass axis along the x and y directions (with respect to the sample), satisfying TM and TE conditions, respectively. The dependence of the out-coupled emission on polarization is clearly seen in these two images. The central lobe in the BFP image (Fig. 7(a)) shows a measured FWHM of 20° for the dye-coated photonic array, compared to 90° for the dye on glass, indicating stronger angular confinement with a side lobe suppression ratio (SLSR) of 2.83 dB. Further details on the quantification are provided in section S12 of the ESI.† This suggests the structure's photonic modes and its angular anisotropic features dictate emission behaviour in angular shaping, which can be tailored through polarization filtering of emitted light to a great extent. The detailed description of all the high-intensity bands observed in the BFP images is discussed in section S11 of the ESI.† Thus, the BFP imaging shown above not only offers clear proof of mode-specific coupling between the emitters and the photonic array but also sets the stage for a variety of advanced applications, including optical diagnostics, fluorescence polarization microscopy,64,65 biosensing, and the design of very directional light-emitting diodes (LEDs).10
While the PL enhancement observed in our structure closely matches the calculated LDOS enhancement, it is important to note that, in general, PL enhancement can differ from LDOS enhancement due to additional factors such as light extraction efficiency, nonradiative losses, and the specifics of experimental detection. Notably, this work provides a comprehensive quantitative demonstration of spatially uniform optical amplification and directional emission in large-area and industrially scalable photonic arrays, thereby linking large-scale nanofabrication with practical photonic applications.
Footnote |
† Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d5nr02160j |
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