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Optical Engineering of Colloidal Quantum Dot Films: From Effective-Medium to Device Architectures
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  • Jugyoung Kim
    Jugyoung Kim
    Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
    More by Jugyoung Kim
  • Ha-Chi V. Tran
    Ha-Chi V. Tran
    Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
  • Sohee Jeong*
    Sohee Jeong
    Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
    Department of Future Energy Engineering, Sungkyunkwan University, Suwon 16419, Republic of Korea
    Sungkyunkwan Institute of Energy Science and Technology, Suwon 16419, Republic of Korea
    *Email: [email protected]
    More by Sohee Jeong
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ACS Applied Optical Materials

Cite this: ACS Appl. Opt. Mater. 2025, 3, 11, 2475–2485
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https://doi.org/10.1021/acsaom.5c00465
Published November 17, 2025

Copyright © 2025 American Chemical Society. This publication is licensed under these Terms of Use.

Abstract

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Colloidal quantum dots (CQDs) are promising candidates for next-generation infrared optoelectronics. While maximizing external quantum efficiency─a key figure of merit for photodetectors and photovoltaics─requires both enhanced light absorption and efficient carrier extraction, the former has received comparatively less attention. This work presents a framework for tailoring the optical properties of CQD films to engineer enhanced absorption in optoelectronic devices. Using effective-medium theory, we discuss how the complex refractive index of CQD films can be modeled and how their optical constants can be systematically related to the quantum dot size, ligand length, and shape. Employing transfer-matrix method calculations, we show how to optimize multilayer stacks by utilizing Fabry–Pérot resonances to maximize absorption. We also present methods to mitigate parasitic losses that limit the absorptance. This framework helps to diagnose whether the device performance is limited by absorption or by carrier extraction and guides research directions toward overcoming these limits. Finally, we discuss the limitations of current theoretical models and propose future directions for extending these principles to emerging optoelectronic applications.

This publication is licensed for personal use by The American Chemical Society.

Copyright © 2025 American Chemical Society

Introduction

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The infrared (IR) spectral region underpins high-impact technologies, from tandem photovoltaics (PVs) to photodetectors (PDs). In tandem solar cells, IR absorbers function as narrow-band-gap bottom cells that enable power conversion efficiencies (PCEs) beyond the single-junction Shockley–Queisser limit. (1,2) Meanwhile, short-wavelength infrared (SWIR) PDs exploit low scattering, deep penetration, and eye-safe illumination to meet emerging demands in automotive sensing, biosensing, and surveillance. (3,4) However, current IR materials─InGaAs and HgCdTe─remain hampered by high production costs and complex processing, limiting scalable implementation. (5)
Colloidal quantum dots (CQDs) offer a promising alternative for IR optoelectronics due to their size-tunable band gap and solution processability, allowing for scalable fabrication and direct integration on various substrates. (6,7) In CQD solids, the high-surface-to-volume ratio enables precise control of electrical and optical properties through surface modification. (8) While extensive studies have shown that surface engineering can effectively tailor electrical properties such as the charge-carrier mobility (9−13) and energy-level alignment, (14−17) systematic strategies to manipulate optical constants remain relatively unexplored. This gap arises from the complex interplay of processing conditions, surface chemistry, and the CQD core size. The optical response of CQD films reflects the combined contributions of the inorganic cores, organic ligands, and voids. Effective-medium theory (EMT) provides a systematic framework to connect constituent dielectric functions and volume fractions to the complex refractive index of a film, serving as an input to optical simulations for CQD device design. (18,19)
CQD-based IR devices typically employ photodiode architectures, in which charge extraction is governed by drift–diffusion transport. (20−23) The external quantum efficiency (EQE)─a key figure of merit in PVs and PDs─reflects both photogeneration and extraction. Recent advances have emphasized extraction; however, maximizing the EQE also requires increased active layer absorptance. In practice, short carrier-diffusion lengths constrain the active-layer thickness, leading to an optical–electrical trade-off. (24) Under this constraint, optimization approaches have largely relied on empirical methods. (25) In addition to increasing light in-coupling, (26−28) plasmonic effects (29,30) and ray-optical strategies (31−33) (diffraction- or scattering-based light trapping) have been explored to increase the optical path length and field intensity, but they often add fabrication complexity. Meanwhile, optical engineering for CQD-based IR devices aims to achieve targeted absorptance enhancement at specific wavelengths, for which optical-cavity tuning─exploiting the multilayer architecture of CQD devices─can provide a straightforward and scalable route through controlled layer thickness. The corresponding internal field distributions can be predicted by optical simulations. Within this optical-cavity framework, optical engineering quantifies active layer absorptance and decouples photogeneration from extraction contributions in the EQE. This approach enables systematic diagnosis of performance-limiting mechanisms and provides design guidelines for CQD optoelectronics.
This Spotlight on Applications provides a structured overview of CQD film optical properties and device-engineering strategies for CQD optoelectronics. We employ EMT to formalize the optical response of CQD films and illustrate how three experimentally accessible parameters─core size, ligand length, and particle shape─influence the packing density and the resulting optical constants. In addition, we describe three cavity-based strategies that can increase active-layer absorptance and, consequently, EQE in CQD devices: (i) active-layer thickness optimization, (ii) optical-spacer engineering, and (iii) transparent-electrode design. Together, these elements provide guidance for the design of high-performance CQD-based IR PVs and SWIR PDs.

Modeling the Optical Response of CQD Thin Films: An EMT

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At the microscopic scale, a CQD film is a heterogeneous assembly of quantum dot cores, organic ligands, and interparticle voids. Despite this structural complexity, the optical response can be captured using EMT, a well-established framework for describing composite materials. Given that the quantum dot diameters (2–10 nm) are orders of magnitude smaller than the operating wavelengths (400–1500 nm), the film satisfies the quasi-static approximation and can be treated as a homogeneous effective medium. (34) In EMT, the dielectric functions and volume fractions of each constituent are combined through a mixing relationship to produce the film’s effective dielectric function (ε̃eff = ε′eff + eff″). This approach provides a direct link between the microscopic constituent properties and the macroscopic optical response.
As illustrated in Figure 1, EMT transforms the complex heterogeneous structure of a CQD film into a simplified homogeneous medium. The top panel depicts the film microstructure, including inorganic cores, ligands, and voids. The lower panel shows the EMT replacement by a homogeneous medium characterized by ε̃eff. In this framework, CQD cores are treated as inclusions, and the surrounding ligands and voids act as the host medium. The dielectric functions of the core (ε̃core) and host (ε̃h) describe their respective optical properties, while structural features (size, shape, and spatial arrangement) are represented through volume fractions. Specifically, the core volume fraction (fcore) can be estimated using a hard-sphere model. (35,36) Assuming a rigid ligand shell and random close packing of monodisperse spheres with packing fraction (PF) ≈ 0.64, (37)
fcore=(rcorercore+lligand)3PF
(1)
where rcore is the core radius and lligand is the ligand length.

Figure 1

Figure 1. Effective-medium view of CQD films. Top: A heterogeneous CQD film comprises inorganic CQD cores, organic ligands, and interparticle voids; microstructural attributes─core size/shape and interdot spacing─govern packing. Bottom: In EMT, the film is replaced by a homogeneous medium with complex permittivity (ε̃eff); the CQD cores (ε̃core) act as inclusions embedded in a host of ligands and voids (ε̃h). The volume fractions fcore and fh encode the microstructure; the panels on the right illustrate different volume fractions.

The effective dielectric function of a CQD film can be described by two widely used EMT models, each suited to different structural configurations. (38) The Maxwell–Garnett model, valid for spherical inclusions dispersed in a host matrix at low volume fractions, is given by
ε~effε~hε~eff+2ε~h=fcoreε~coreε~hε~core+2ε~h
(2)
Alternatively, when the volume fractions of inclusion and host are comparable, the Bruggeman model applies and is expressed as
fcoreε~coreε~effε~core+2ε~eff+fhε~hε~effε~h+2ε~eff=0
(3)
where fh = 1 – fcore is the volume fraction of the host material. In practice, the choice between these models is determined by the volume fraction. For densely packed structures, where the host–inclusion distinction is diminished, the Bruggeman model is more appropriate, given its symmetric treatment of both constituents.

Experimental Determination of the Effective Optical Constants in CQD Thin Films

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Spectroscopic ellipsometry nondestructively determines the CQD film thickness and effective optical constants over a broad spectral range. (39−41) The polarization change upon reflection is measured as Ψ and Δ, defined through the complex reflection-coefficient ratio (ρ)
ρrprs=tan(Ψ)eiΔ
(4)
where rp and rs are the complex reflection coefficients for p and s polarizations, respectively. Ψ and Δ are globally fitted with a multilayer model at multiple angles to yield the film’s effective dielectric function (ε̃eff = ε′eff + iε″eff) and thickness. Conversion then gives the effective complex refractive index (Ñeff = neff + iκeff) and the absorption coefficient α=4πκλ, where λ is the wavelength. Ellipsometry thus complements EMT: EMT predicts trends from microscopic parameters (core size, ligand length, and particle shape) via changes in the volume fraction, whereas ellipsometry supplies the measured complex refractive index of the CQD film to validate these predicted trends, and furthermore provieds input for optical-cavity designs in device simulations.

Effective-Medium Perspective on CQD Film Optical Constants

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This section applies EMT to interpret experimental results on how the core–shell structure, particle size, surface ligands, and particle shape influence ε̃eff and the complex refractive index of CQD thin films.
Dement et al. (2018) (35) compared complex refractive indices extracted of CdSe cores and CdSe/CdS core–shell nanocrystals dispersed in solution (Figure 2a) with those of the corresponding thin films measured by spectroscopic ellipsometry (Figure 2b). The effective optical constants of films were generally smaller than those of the isolated nanocrystals. This behavior is consistent with EMT because thin films incorporate not only the inorganic core–shell material but also surface ligands and voids. Given that bulk CdS has a refractive index lower than that of CdSe, increasing the CdS shell fraction leads to a systematic reduction in the overall film refractive index. The extinction coefficient (κ) exhibits pronounced composition dependence at wavelengths longer than the shell band gap, where absorption is primarily governed by the CdS shell, whereas at shorter wavelengths, the variation is more gradual due to contributions from both the core and shell. Notably, the pure CdSe core film shows a lower complex refractive index than the CdSe/2CdS core–shell film, ascribed to its reduced inorganic packing density.

Figure 2

Figure 2. Complex refractive index of the CdSe cores and CdSe/CdS core–shell nanocrystals extracted in solution (a) and thin films (b). Adapted with permission from ref (35). Copyright 2018 American Chemical Society. The average refractive index of PbS CQD films from ellipsometry (symbols) and fNC (blue), obtained by fitting the ellipsometry data using the Bruggeman model or by a hard-sphere model (orange), plotted as a function of the PbS CQD excitonic peak (c) and surface ligand (d). Adapted with permission from ref (38). Copyright 2022 Royal Society of Chemistry. Real part of the effective dielectric function (e) and transfer curve (f) for InAs CQD films composed of tetrahedra (red) or spheres (blue) with identical particle volume (32 nm3). Adapted from ref (42) under the CC BY-NC-ND license. Copyright 2024 American Chemical Society.

When the core dielectric function is extracted in solution, solvent- and ligand-induced dielectric screenings may be included. In Figure 2c, Chehaibou et al. (2022) (38) combined the intrinsic dielectric function of PbS cores─calculated using a tight-binding (TB) model─with EMT to quantify the dependence of both the nanocrystal volume fraction (fNC) and effective refractive index on the particle size. The fNC values derived from a hard-sphere model (fNC hard-sphere model, orange line) closely match with those extracted from the fitting ellipsometry data using the Bruggeman model (fNC fitted, blue line), even though the hard-sphere model slightly underestimates the values due to its assumption of rigid, noninterdigitated ligand shells. The average refractive index of PbS CQD films─calculated as the spectrally averaged value of n(λ) over 750–2000 nm─and the volume fraction both increase with the core size, suggesting that larger cores elevate the inorganic volume fraction and, in turn, enhance the effective refractive index of the films. Furthermore, as shown in Figure 2d, the ligand length can also modulate the volume fraction. Replacing long-chain oleate (OA) with shorter ethanedithiol (EDT) or ammonium iodide (NH4I) increases fNC, which, in turn, drives increases in both the refractive index and extinction coefficient.
Shape effects provide an additional optimization parameter. As shown in Figure 2e, tetrahedral and spherical InAs quantum dots of identical volumes exhibit markedly different dielectric functions, with tetrahedral particles displaying higher values. Kim et al. (2024) (42) estimated the volume fractions from GISAXS-derived interdot distances, finding 57.2% for tetrahedral films versus 31.2% for spherical films. The higher packing density of tetrahedral quantum dots corresponds to both enhanced dielectric function (Figure 2e) and improved carrier mobility (Figure 2f), indicating that shape engineering represents a powerful strategy for optimizing the device performance.
In summary, the optical response of CQD films is governed primarily by the inorganic-core dielectric function and the nanocrystal volume fraction. Within EMT, these key descriptors provide a quantitative basis for interpreting the dependencies of composition, ligand, and shape, thereby enabling a comprehensive understanding of the spectral response.

Optical-Cavity Engineering in CQD Photodiodes for IR Optoelectronics

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The transition from single-layer films to full device architecture requires explicit consideration of interlayer correlations that also strongly influence the optical and electronic behavior. The multilayer structure of CQD photodiodes, as shown in Figure 3a, typically includes a transparent conducting oxide (TCO), an electron-transport layer (ETL), a CQD absorber, a hole-transport layer (HTL), and a metal electrode, inherently forming a cavity between the highly reflective metal electrode and the partially reflective TCO. This Fabry–Pérot (FP) resonance strongly modulates the device absorption spectrum, and by adjustment of the optical path length of individual layers, the cavity can be tuned to realize wavelength-selective responses in both solar cells and PDs.

Figure 3

Figure 3. (a) Multilayer CQD photodiode (TCO/ETL/CQD absorber/HTL/metal) forming a FP cavity. (b) TMM: each layer with thickness di and complex index Ñi represented by Mi. The total transfer matrix (M) relates to the incident and reflected fields. (c) Simulated electric-field intensity (|E| 2) vs wavelength (1100–1600 nm) and position. A resonance near 1.3 μm concentrates the field in the CQD layer. (d) Calculated nanocrystal absorption vs CQD film thickness and wavelength. Slanted bands are FP resonances. Adapted with permission from ref (38). Copyright 2022 Royal Society of Chemistry.

The optical behavior of this cavity can be predicted and optimized with the transfer-matrix method (TMM), a widely used optical modeling tool. (43−45) TMM describes electromagnetic-wave propagation through a multilayer stack by representing each layer as a 2 × 2 transfer matrix that combines interfacial reflection/transmission and propagation. As illustrated in Figure 3b, the overall optical response is obtained by sequentially multiplying the individual transfer matrixes (M1,M2, ..., Mn). Each matrix accounts for two key processes: interfacial reflection and transmission, described by Fresnel coefficients, and wave propagation through the layer─phase accumulation and attenuation determined by its complex refractive index (Ñ) and thickness (d). The reflected field amplitude (ref) is computed from the incident field amplitude (inc) through the total transfer matrix (M). This enables calculation of the device reflectance, transmittance, and, critically, spatial distribution of optical fields. Figure 3c illustrates the 2D electric-field intensity distribution within a CQD photodiode from 1100 to 1600 nm. A strong resonance is observed at ≈1300 nm, where constructive interference between forward- and backward-propagating waves leads to pronounced field enhancement in the CQD absorber. When the absorber thickness is adjusted so that a cavity resonance coincides with the first excitonic peak, the absorptance at that peak can be significantly enhanced.
The practical use of TMM is shown in Figure 3d, which maps the dependence of the wavelength and thickness on the absorptance of a SWIR PbS CQD photodiode. (38) The nearly horizontal band corresponds to the first excitonic transition, while the tilted bands arise from FP resonances. These resonances shift periodically with a spacing of Δd ≈ λ/(2neff), where λ is the free-space wavelength and neff is the effective refractive index of the cavity, causing a nonmonotonic variation in absorptance with thickness─specific thicknesses yield stronger absorption than thicker counterparts due to constructive interference. TMM thus identifies the optimal absorber thicknesses for target wavelengths, producing an absorptance map that, under the unity-carrier-collection assumption, serves as an upper bound for the EQE. (46) These simulations provide the foundation for the systematic device optimization strategies detailed in the following sections.

Optimizing the Thickness of the CQD Absorbing Layer for Enhanced Device Performance

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The absorptance of PbS CQD SWIR PDs was quantified in an indium–tin oxide (ITO)/TiO2/PbS-NH4I/PbS-EDT/Au structure, as shown in Figure 3d. (38) TMM simulations revealed that an optimized absorber thickness (≈330 nm) yields ≈80% absorptance at the first excitonic peak (≈1200 nm). The calculation further revealed a nonmonotonic dependence of the absorptance on the active-layer thickness due to FP interference. Importantly, this simulation result indicates that the remaining 20% optical loss originates from parasitic absorption in the TCO and metal electrodes, thereby establishing a fundamental limit for this structure. Tran et al. (2025) (47) measured the EQE for an ITO/ZnO/PbS-NH4I/PbS-EDT/Au stack while varying the active-layer thickness from 300 to 570 nm and observed ≈80% EQE near 1550 nm (Figure 4a), in agreement with their TMM result at that wavelength. Taken together, these results show that optical simulations quantitatively reproduce thickness-dependent resonances and peak responses across device architectures and target wavelengths.

Figure 4

Figure 4. Thickness optimization of CQD absorbers. (a) PbS SWIR PD: TMM absorptance at the excitonic peak vs active-layer thickness (black) with measured EQE at 1550 nm under −2 V (red). Data from ref (47). (b) Micrometer-thick PbS CQD solar cell: EQE (purple) with the AM1.5G spectrum (gray). Adapted with permission from ref (50). Copyright 2020 American Chemical Society. (c) InAs NIR PD: TMM absorptance vs film thickness with representative reported EQEs (colored symbols). (d) Expected EQE from TMM (black) vs measured EQE (red circles) at 940 nm. (e) Thickness and bias dependent EQE (f) Specific detectivity at −1 V vs thickness (inset, EQE spectra). Adapted with permission from ref (51). Copyright 2024 Wiley-VCH GMbH.

Unlike perovskite or organic optoelectronics, (48,49) where transparent electrodes exhibit negligible reflection in the visible region, CQD photodiodes operating in the SWIR show a much stronger thickness dependence. This perspective suggests that such behavior may originate from the increased refractive index contrast between the TCO and the internal layers, which enhances the cavity finesse and strengthens the FP resonance formed between the two electrodes. This effect, together with optical losses within the internal layers and electrodes, is expected to shape the overall absorptance behavior.
Experimentally, Fan et al. (2020) (50) investigated a PbS CQD solar cell with an ITO/ZnO/PbS-PbX/PbS-EDT/Au structure and confirmed that the FP resonance peaks red-shifted with increasing active-layer thickness. To enhance IR harvesting, micrometer-thick CQD films were successfully fabricated via the blade-coating technique. The device attained a high EQE, approaching 80% at both the first excitonic peak (≈1670 nm) and the nearest FP resonance peak (≈1210 nm) (Figure 4b). Consequently, the device achieved an IR short-circuit current density of 9.81 mA/cm2, representing a 70% improvement over the previously reported values. However, further increases in thickness introduced a trade-off, reducing the IR fill factor (FF) due to enhanced carrier recombination. This suggests that balancing the electrical and optical factors is critical to the design of high-performance devices.
More recently, Shin et al. (2025) (51) conducted optical simulations to examine the performance limitations of Pb-free InAs CQD near-IR (NIR) PDs. The low EQE of previous reports (≈40%) was found to be a result of insufficient absorber-layer thickness. The simulations predicted that an ideal EQE approaching 76% could be reached with an absorber layer thickness of approximately 290 nm (Figure 4c). To validate the prediction, InAs CQD films with thicknesses ranging from 60 to 330 nm were successfully fabricated using a dual-solvent engineering technique, followed by the fabrication of NIR photodiodes based on these films. A comparison of the EQE, measured under a reverse bias sufficient for charge-carrier extraction, with the absorptance values obtained from TMM calculation revealed close consistency between experiment and simulation (Figure 4d). This result validates optical simulation as a reliable tool for predicting the ideal EQE of a device. Leveraging this methodology, this study achieved the highest EQE performance reported to date for InAs CQD PDs.
To extend this optical-engineering framework, Table 1 summarizes the complex refractive indices of PbS and InAs CQDs in the IR range and resonant peak positions and simulated EQE obtained from TMM calculations based on an ITO/ZnO/CQD/MoOx/Au structure. The refractive index dictates the optimal active-layer thickness for optical resonance, while the extinction coefficient affects the achievable EQE. Specifically, the larger complex refractive index of the PbS CQD film at 940 nm results in the resonance peak appearing at a thinner active-layer thickness at the same wavelength, while the slightly lower EQE can be attributed to its smaller absorption coefficient. However, a more comprehensive understanding and further systematic research are necessary to clearly establish the precise relationship between the composition and quantum dot size-dependent optical constants and the resulting device performance.
Table 1. Complex Refractive Indices of PbS and InAs CQDs at a Target Wavelength in the IR Range and the Resonance Peak Positions and Corresponding Simulated EQE Values Obtained from TMM Calculations Based on an ITO/ZnO/CQD/MoOx/Au Structure
     resonance peak positionsimulated EQE
resonance order1st excitonic peak (nm)nκsource1st2nd3rd1st2nd3rd
PbS I9402.8050.107 (51)50220380407381
PbS I12202.7200.149 (38)90310535747363
InAs Br9452.1920.118 (51)70280500527983
InAs Br13242.2190.122in-house130410690657166
Meanwhile, bias-dependent EQE measurement further revealed a depletion of 60–105 nm because a thicker absorber layer thickness required a higher applied bias to reach saturation (Figure 4e). The specific detectivity (D*) of the InAs CQD PD was then determined from the dark current and the measured EQE at −1 V. The thickness-dependent D* showed an increasing trend as the dark current decreased in the 60–165 nm range. In contrast, in the 250–330 nm range, D* follows the trend of the EQE, achieving a value of 3.1 × 1011 Jones at 290 nm. However, at −3 V, when the EQE was maximized, the D* decreased to 1.3 × 1011 Jones due to the elevated dark current (Figure 4f). This trade-off highlights that an optimal device performance requires balancing signal enhancement (EQE) with noise suppression (dark current) rather than simply maximizing EQE alone. Through optical engineering, this work identifies the performance bottlenecks in InAs CQD PDs and demonstrates the critical importance of a design methodology that integrates both electrical and optical considerations.

Optical-Spacer Engineering for Enhanced CQD Photodiode Performance

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While previous strategies primarily focused on tuning the optical path length through variations in the active-layer thickness, recent studies have shown that device absorptance is also governed by the optical constants and thickness of all functional layers because components such as the ETL and HTL contribute directly to the optical cavity. Chehaibou et al. (2022) reported that the total thickness comprising both n-type and p-type PbS CQD films affects the resonant condition. (38) Building on this insight, subsequent studies have employed charge-transport layers as “optical spacers” to tailor the internal electric-field distribution and enhance the device performance. Tran et al. (2025) introduced a molybdenum oxide (MoOx) layer as an injection-blocking layer (IBL) between PbS-EDT and the Au electrode to suppress dark current. (47) Optical simulations further confirmed that increasing the MoOx thickness reduced the optimal active layer thickness required to maximize EQE at 1550 nm (Figure 5a), underscoring the dual function of the MoOx layer as both an electrical barrier and an optical spacer within the cavity. By cooptimization of the active layer thickness with a 40 nm MoOx layer, the PbS CQD PD achieved an EQE of 84%. This strategy reduced the dark current density by a factor of 16, yielding a high D* of 8.6 × 1011 Jones at −1 V (Figure 5b).

Figure 5

Figure 5. Optical-spacer engineering in CQD photodiodes. PbS SWIR PD with a MoOx IBL: (a) Simulated absorptance vs active-layer thickness for MoOx = 0, 10, 25, and 40 nm. (b) Specific detectivity at −1 V and dark current–voltage characteristics (inset) for devices with MoOx (black) and without MoOx (blue). Adapted with permission from ref (47). Copyright 2025 American Chemical Society. InAs CQD IR solar cell with a p-type optical spacer: (c) Simulated EQE vs p-InAs thickness for n-type absorber thicknesses of 90, 110, and 120 nm. 2D electric-field-intensity maps without (d) and with a 30 nm p-InAs layer (e). (f) Measured EQE (solid) for p-InAs thickness = 0, 15, and 30 nm and calculated integrated Jsc. Adapted with permission from ref (52). Copyright 2024 Wiley-VCH GMbH.

Park et al. (2025) presented a Pb-free InAs CQD IR solar cell with a homojunction architecture that uses both n-type and p-type InAs CQD films to block electron backflow and facilitate hole extraction from the n-type layer. (52) This p-type layer served dual roles as an electrical barrier and an optical spacer that tunes the device resonance condition. Optical simulations predicted significant performance improvements for the thin-absorber architecture. While the optimal thickness for a device without a p-type layer was 140 nm, adding a 30 nm p-type layer to a 110 nm n-type absorber was predicted to increase the ideal EQE from 20% to 55% (Figure 5c). By modulation of the p-type layer thickness to tune the optical path length, the electric-field enhancement can be localized within the active layer, thereby increasing the device absorptance. This phenomenon is supported by electric-field-distribution simulations both without (Figure 5d) and with (Figure 5e) a p-type InAs CQD layer. This prediction was experimentally verified: by inserting an optimized 30 nm p-type layer─a thickness that balances optical gains against the FF losses seen above 40 nm─the peak EQE was boosted from 28% to 38%, inducing a redshift (Figure 5f). Leveraging the dual electrical and optical roles of the p-type layer, the optimized InAs CQD IR solar cell achieved a PCE of 2.00% under AM1.5G and 0.27% with a Si-filtered spectrum. These values significantly surpassed the control device without the p-type layer (0.28% and 0.03%, respectively). This study demonstrates the necessity of a comprehensive device-design strategy for photodiodes that considers not only the electrical and optical roles of the active layer but also those of other functional layers. These results highlight the importance of developing CQD films that offer combined control over both the electrical and optical properties, which is a crucial aspect of designing advanced optoelectronic devices.

Minimizing Parasitic Absorption through Advanced Electrode Engineering

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Parasitic absorption in ITO remains a major limitation of the absorptance of IR CQD photodiodes. This challenge can be addressed by enhancing the transmittance of ITO through optimized material properties and processing conditions, as well as by employing advanced transparent-electrode designs such as distributed Bragg reflectors (DBRs) and asymmetric electrode architectures. Employing a SiNx/SiO2 dielectric stack as a DBR front mirror and optimizing the active-layer thickness (Figure 6a) allow precise control of the front mirror reflectivity and central wavelength. Ouellette et al. (2016) demonstrated enhanced IR absorption via tailored optical resonances and achieved a 56% enhancement in the IR PCE relative to an ITO-based control device (Figure 6b). (53) Separately, Baek et al. (2018) developed an asymmetric multilayer electrode with an ITO/Ag/ZnO (IMZ) stack, which minimizes parasitic absorption while maintaining a low sheet resistance of ≈10 Ω sq–1. (54) As shown in Figure 6c, the IMZ structure maintains a high transmittance in the IR region. PbS CQD IR solar cells fabricated with this IMZ electrode exhibited an approximately 2-fold increase in IR absorption compared to an ITO-based device, resulting in a high EQE of 70% at ≈1250 nm (Figure 6d). These studies demonstrate that advanced electrode engineering effectively minimizes parasitic absorption while maintaining electrical conductivity, enabling high-performance IR CQD optoelectronics.

Figure 6

Figure 6. Advanced electrode designs for IR CQD solar cells. DBR cavity: (a) Schematic of reflective top contact and a DBR mirror contact, forming an optical cavity that enhances IR multipass. (b) EQE of the cavity device (red) versus a control without the cavity (black), showing enhancement near 1.3 μm. Adapted with permission from ref (53). Copyright 2016 American Chemical Society. Transparent IMZ electrode: (c) Transmittance of the IMZ asymmetric multilayer (red) compared with ITO (black dashed) over 1000–1800 nm at comparable sheet resistance (≈10 Ω sq–1); inset: IMZ stack. (d) EQE with ITO (black dashed), IMZ without Ag (yellow), and IMZ (red), demonstrating performance gains from the multilayer electrode. Adapted with permission from ref (54). Copyright 2018 American Chemical Society.

Conclusion and Outlook

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This Spotlight on Applications presents a systematic analysis of the optical properties of CQD thin films and optical-engineering strategies for CQD optoelectronics. EMT serves as a key analytical tool, providing a practical approach for determining the effective complex refractive index of CQD films by linking the constituents’ dielectric functions and volume fractions to the film-level optical constants. Three experimentally tunable variables─core size, ligand length, and particle shape─are identified as primary determinants of the volume fraction and, by extension, the effective complex refractive index. Leveraging experimentally measured optical constants, this analysis delineates optical-engineering strategies that exploit the FP cavity effects in multilayer stacks. These strategies─including active-layer thickness tuning, optical-spacer engineering, and electrode design─enhance absorptance and approach theoretical EQE limits with negligible parastic losses.

Challenges and Opportunities in CQD Optical Characterization

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TB calculations offer a powerful approach for predicting quantum dot core dielectric functions, which govern the spectral position and magnitude of absorption features, thereby establishing a direct link between the calculated electronic structure and measurable optical properties. (55−57) While recent reports have provided broader insights into the optical properties of various CQD compositions, (18) experimental validation remains limited. Furthermore, analyses linking TB models with EMT have focused primarily on PbS and HgTe CQDs, (38,58) restricting our understanding of how complex refractive indices vary with the core size and ligand length across different compositions. With the rapid advances in RoHS-compliant materials, such as InAs and InSb CQDs, for optoelectronic devices, it is crucial to extend these analyses to emerging IR materials. (59−61) Systematic cross-composition comparisons─beyond single-composition case studies─will fundamentally advance our knowledge of IR materials and their device-relevant optical behavior.
Additionally, when transitioning from CQDs in solution to solid films and as the interparticle distance decreases within the films, a redshift in the absorption spectrum is commonly observed. (11,62,63) Although the origin of this shift is still being investigated, it is often attributed to polarization effects and electronic coupling between adjacent quantum dots. (64−68) However, the Bruggeman model, which simply averages dielectric functions based on volume fraction, does not completely account for such interparticle interaction in CQD films. While classical EMT can approximate local dielectric screening effects, (69) it does not fully capture polarization effect. Extended models (70−72) that incorporate dipole–dipole interactions, such as the coherent potential approximation or the coupled-dipole model, have been proposed; however, they generally rely on numerical self-consistent solutions rather than analytical forms. Therefore, a complete EMT framework capturing both polarization and electronic coupling effects in CQD films requires further development, and future models should aim to incorporate interparticle interactions into the dielectric averaging framework to more accurately describe the collective optical behavior of CQD assemblies.

Expanding CQD Applications through Advanced Photonic Architecture

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In multilayer CQD photodiodes, optical engineering strategies that maximize the absorptance through cavity effects have been widely explored. However, the current device efficiency remains limited by parasitic absorption in transparent electrodes, restricting the maximum absorptance to approximately 80%. Strategies such as reducing electrode absorption and optimizing the multilayer stack design are expected to overcome this limitation and approach ideal EQE values.
Beyond conventional photodiode architectures, wavelength-selective designs─successfully demonstrated in organic materials─present promising opportunities for CQD devices. These structures enable narrowband detection without external filters, potentially improving signal-to-noise ratios through effective background suppression. (73−75) Moreover, the tunable refractive index of CQD films makes them particularly suitable for solution-processed photonic structures such as DBRs, (76) facilitating the monolithic integration of optical cavities. (77,78) Along with the advantages of solution processability, these structural innovations open new avenues for CQD technologies─enabling filter-free narrowband PDs for precision imaging, biomedical and spectroscopic sensing, and spectrally tailored optical communication, as well as DBR-integrated photonic architectures for both light–matter interaction engineering and efficiency enhancement in light-emitting devices─thereby bridging CQD optoelectronics with emerging quantum photonic platforms. (79,80)

Author Information

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  • Corresponding Author
    • Sohee Jeong - Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of KoreaDepartment of Future Energy Engineering, Sungkyunkwan University, Suwon 16419, Republic of KoreaSungkyunkwan Institute of Energy Science and Technology, Suwon 16419, Republic of KoreaOrcidhttps://orcid.org/0000-0002-9863-1374 Email: [email protected]
  • Authors
    • Jugyoung Kim - Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
    • Ha-Chi V. Tran - Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea
  • Author Contributions

    The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.

  • Funding

    This research was supported by the National Research Foundation, funded by the Ministry of Science and ICT (RS-2022-NR070449 and RS-2024-00444458). It was also supported by Grants RS-2022-00144108 and RS-2024-00418086, funded by the Ministry of Trade, Industry, and Energy of the Korean Government.

  • Notes
    The authors declare no competing financial interest.

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  • Abstract

    Figure 1

    Figure 1. Effective-medium view of CQD films. Top: A heterogeneous CQD film comprises inorganic CQD cores, organic ligands, and interparticle voids; microstructural attributes─core size/shape and interdot spacing─govern packing. Bottom: In EMT, the film is replaced by a homogeneous medium with complex permittivity (ε̃eff); the CQD cores (ε̃core) act as inclusions embedded in a host of ligands and voids (ε̃h). The volume fractions fcore and fh encode the microstructure; the panels on the right illustrate different volume fractions.

    Figure 2

    Figure 2. Complex refractive index of the CdSe cores and CdSe/CdS core–shell nanocrystals extracted in solution (a) and thin films (b). Adapted with permission from ref (35). Copyright 2018 American Chemical Society. The average refractive index of PbS CQD films from ellipsometry (symbols) and fNC (blue), obtained by fitting the ellipsometry data using the Bruggeman model or by a hard-sphere model (orange), plotted as a function of the PbS CQD excitonic peak (c) and surface ligand (d). Adapted with permission from ref (38). Copyright 2022 Royal Society of Chemistry. Real part of the effective dielectric function (e) and transfer curve (f) for InAs CQD films composed of tetrahedra (red) or spheres (blue) with identical particle volume (32 nm3). Adapted from ref (42) under the CC BY-NC-ND license. Copyright 2024 American Chemical Society.

    Figure 3

    Figure 3. (a) Multilayer CQD photodiode (TCO/ETL/CQD absorber/HTL/metal) forming a FP cavity. (b) TMM: each layer with thickness di and complex index Ñi represented by Mi. The total transfer matrix (M) relates to the incident and reflected fields. (c) Simulated electric-field intensity (|E| 2) vs wavelength (1100–1600 nm) and position. A resonance near 1.3 μm concentrates the field in the CQD layer. (d) Calculated nanocrystal absorption vs CQD film thickness and wavelength. Slanted bands are FP resonances. Adapted with permission from ref (38). Copyright 2022 Royal Society of Chemistry.

    Figure 4

    Figure 4. Thickness optimization of CQD absorbers. (a) PbS SWIR PD: TMM absorptance at the excitonic peak vs active-layer thickness (black) with measured EQE at 1550 nm under −2 V (red). Data from ref (47). (b) Micrometer-thick PbS CQD solar cell: EQE (purple) with the AM1.5G spectrum (gray). Adapted with permission from ref (50). Copyright 2020 American Chemical Society. (c) InAs NIR PD: TMM absorptance vs film thickness with representative reported EQEs (colored symbols). (d) Expected EQE from TMM (black) vs measured EQE (red circles) at 940 nm. (e) Thickness and bias dependent EQE (f) Specific detectivity at −1 V vs thickness (inset, EQE spectra). Adapted with permission from ref (51). Copyright 2024 Wiley-VCH GMbH.

    Figure 5

    Figure 5. Optical-spacer engineering in CQD photodiodes. PbS SWIR PD with a MoOx IBL: (a) Simulated absorptance vs active-layer thickness for MoOx = 0, 10, 25, and 40 nm. (b) Specific detectivity at −1 V and dark current–voltage characteristics (inset) for devices with MoOx (black) and without MoOx (blue). Adapted with permission from ref (47). Copyright 2025 American Chemical Society. InAs CQD IR solar cell with a p-type optical spacer: (c) Simulated EQE vs p-InAs thickness for n-type absorber thicknesses of 90, 110, and 120 nm. 2D electric-field-intensity maps without (d) and with a 30 nm p-InAs layer (e). (f) Measured EQE (solid) for p-InAs thickness = 0, 15, and 30 nm and calculated integrated Jsc. Adapted with permission from ref (52). Copyright 2024 Wiley-VCH GMbH.

    Figure 6

    Figure 6. Advanced electrode designs for IR CQD solar cells. DBR cavity: (a) Schematic of reflective top contact and a DBR mirror contact, forming an optical cavity that enhances IR multipass. (b) EQE of the cavity device (red) versus a control without the cavity (black), showing enhancement near 1.3 μm. Adapted with permission from ref (53). Copyright 2016 American Chemical Society. Transparent IMZ electrode: (c) Transmittance of the IMZ asymmetric multilayer (red) compared with ITO (black dashed) over 1000–1800 nm at comparable sheet resistance (≈10 Ω sq–1); inset: IMZ stack. (d) EQE with ITO (black dashed), IMZ without Ag (yellow), and IMZ (red), demonstrating performance gains from the multilayer electrode. Adapted with permission from ref (54). Copyright 2018 American Chemical Society.

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