Optical cavities with excellent resonance and light confinement activities play crucial roles in light generation, modulation, detection, sensing, and storage for the realization of optical functional devices, integrations, and communications.1
Advanced Photonics, Volume. 6, Issue 3, 036001(2024)
Optical cavities play crucial roles in enhanced light–matter interaction, light control, and optical communications, but their dimensions are limited by the material property and operating wavelength. Ultrathin planar cavities are urgently in demand for large-area and integrated optical devices. However, extremely reducing the planar cavity dimension is a critical challenge, especially at telecommunication wavelengths. Herein, we demonstrate a type of ultrathin cavities based on large-area grown Bi2Te3 topological insulator (TI) nanofilms, which present distinct optical resonance in the near-infrared region. The result shows that the Bi2Te3 TI material presents ultrahigh refractive indices of >6 at telecommunication wavelengths. The cavity thickness can approach 1/20 of the resonance wavelength, superior to those of planar cavities based on conventional Si and Ge high refractive index materials. Moreover, we observed an analog of the electromagnetically induced transparency (EIT) effect at telecommunication wavelengths by depositing the cavity on a photonic crystal. The EIT-like behavior is derived from the destructive interference coupling between the nanocavity resonance and Tamm plasmons. The spectral response depends on the nanocavity thickness, whose adjustment enables the generation of obvious Fano resonance. The experiments agree well with the simulations. This work will open a new door for ultrathin cavities and applications of TI materials in light control and devices.
1 Introduction
Optical cavities with excellent resonance and light confinement activities play crucial roles in light generation, modulation, detection, sensing, and storage for the realization of optical functional devices, integrations, and communications.1
Electromagnetically induced transparency (EIT) is a counterintuitive quantum interference effect occurring in atomic systems.25 The EIT effect acts as an essential role in modern optical physics due to its significant applications in optical data storage, optical switching, and enhanced light nonlinearities.26 Even so, the practical applications of atomic EIT are limited by the rigorous requirements of low temperature or stable gas lasing conditions.27 Fortunately, the analogies to atomic EIT were observed in conventional optical cavities, such as photonic crystal cavities,28 whispering-gallery-mode cavities,29,30 and metallic cavities.31
Herein, we reported a type of ultrathin planar cavities based on the large-area grown TI nanofilms, which possess obvious optical resonance in the near-infrared region. The experimental results demonstrate that the TI material presents ultrahigh refractive index at near-infrared wavelengths, contributing to the realization of optical cavities that are tens of nanometers in thickness. The TI material-based nanocavity thickness is of resonance wavelength (), much thinner than those of cavities based on the conventional HRI Si and Ge materials. We also experimentally observed an analogy to atomic EIT at telecommunication wavelengths by depositing the nanocavity onto a one-dimensional (1D) photonic crystal. A transparency window distinctly appears in the original cavity-induced resonance absorption spectrum owing to the coupling between the nanocavity resonance and Tamm plasmons. The spectral profile relies on the cavity thickness and can evolve to an asymmetric Fano resonance line shape. The experimental results agree well with the simulations. This work will pave a new pathway for ultrathin optical cavities as well as the applications of TI materials in the mimicking of EIT and optoelectronic devices.
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2 Results
Figure 1(a) shows the 3D diagram of the cavity with a TI material nanofilm coating on a metallic layer. To explore the optical properties, we fabricated the TI nanocavity by using a magnetron sputtering (MS) technique (see Appendix). Figure 1(b) depicts an angle-tilted cross-sectional scanning electron microscopic (SEM) image of a nanocavity with the and silver nanofilms deposited on a substrate. and denote the thicknesses of and silver films, respectively. A 2-nm layer was deposited to isolate the silver and films for avoiding the formation of the Schottky barrier and charge transport.35 The optical and top-view SEM images reveal the large area and good flatness properties of MS-grown nanofilms, respectively (see Fig. S1 in the Supplementary Material). Compared with the pulsed laser deposition, the MS technique enables the large-area growth of relatively flat films.36 The MS method also presents the better flatness and higher growth rate for fabricating films when compared with the atomic layer deposition.37Figure 1(c) depicts the absorption spectrum of a 42-nm TI film on a 30-nm silver layer (i.e., and ). The TI thickness can be clarified using the atomic force microscope (AFM) measurement (see Fig. S2 in the Supplementary Material). We measured the reflection, transmission, and absorption spectra of a TI nanocavity using a spectrophotometer (see Appendix). In Fig. S3 in the Supplementary Material, a distinct reflection dip appears at wavelength (i.e., ) for the cavity with a thickness of , which is derived from the Fabry–Perot resonance in the asymmetric nanocavity. Here, the flat silver film with a large area can reflect a part of the incident light. The silver-reflected light will generate destructive interference with directly reflected light from the TI layer around the resonance wavelength.13 Thus, the reflection light of the cavity can be effectively suppressed. The cavity thickness of is ultrathin, according to the reported cavities.10,38,39 The optical loss of TI gives rise to strong resonance absorption at a broad wavelength range covering 1100 to 1800 nm, as depicted in Fig. 1(c). Moreover, we proposed to integrate the TI nanocavity onto a 1D photonic crystal, as can be seen in Fig. 1(d). The TI nanocavity was deposited on a photonic crystal with alternately stacked and layers. The and layers were fabricated using electron beam deposition. Figure 1(e) shows the angle-tilted cross-sectional SEM image of a fabricated TI nanocavity/photonic crystal structure. We can see that the photonic crystal has good uniformity with the periodic number . The thicknesses of and layers are 182 and 260 nm, respectively (i.e., and ). Figure 1(f) depicts the absorption spectrum of TI nanocavity/photonic crystal structure with and . A distinct narrow dip appears around 1550 nm wavelength in the absorption spectrum. Thus, the original broad absorption of TI nanocavity exhibits a transparency window at the telecommunication wavelength, which is analogous to the EIT effect in atomic systems.28,29 Meanwhile, we characterized the grown nanofilm using a transmission electron microscope (TEM). Figure 2(a) shows the TEM image of a grown 42-nm TI film transferred on the supporter of a copper microgrid (see Appendix and Note 1 in the Supplementary Material). The chemical composition of nanofilm can be confirmed using the energy-dispersive X-ray (EDX) measurement, which reveals the atomic ratio of (see Fig. S4 in the Supplementary Material). The good quality of can also be verified by the Raman shift spectrum (see Fig. S5 in the Supplementary Material).40Figure 2(b) depicts the selected area electron diffraction (SAED) pattern of nanofilm, which corresponds to the rhombohedral phase.41 It also denotes that the MS-grown nanofilm presents the preferred growth orientation of (015). The high-resolution TEM (HRTEM) image in Fig. 2(c) illustrates multi-orientation atomic lattice arrangements in the nanofilm. The HRTEM image exhibits distinct fringes with some lattice spacing containing 0.321 and 0.220 nm, corresponding to the (015) and (110) planes of , respectively. The continuous rings of sharp diffraction pattern and atomic lattice arrangements reveal the polycrystalline nature of the nanofilm. We measured the optical constant of TI using a spectroscopic ellipsometer (see Appendix and Note 2 in the Supplementary Material). To differentiate the surface and bulk states, the ellipsometer-measured results can be fitted with the layer-on-bulk model.42,43 The surface and bulk were fitted with the Drude and Tauc–Lorentz dispersion relations, respectively.42
Figure 1.TI structures and absorption spectra. (a) 3D diagram of the ultrathin nanocavity with a TI nanofilm coated on a metallic layer. (b) Angle-tilted cross-sectional SEM image of a
Figure 2.Material characterization and optical constants of
Subsequently, we measured the absorption spectra of TI nanocavities with different thicknesses. As shown in Fig. 3(a), the resonant absorption wavelength presents a redshift in the near-infrared region as increases from 30 to 52 nm. Simultaneously, the absorption peak possesses an obvious rise. To verify the experimental results, the absorption spectra were theoretically calculated using the transfer matrix method (see Fig. S6 and Note 3 in the Supplementary Material).48 In the calculations, we employed the measured complex refractive indices of the TI surface and bulk in Figs. 2(e) and 2(f) as well as the measured optical constants of silver film in Fig. S7 in the Supplementary Material. As depicted in Fig. 3(b), there exists a nearly linear relation between the absorption peak wavelength and TI thickness. As mentioned above, the TI nanocavity thickness is of the resonance wavelength. Moreover, we simulated the spectral response and field distributions of the TI nanocavities using the finite-difference time-domain (FDTD) method (see Appendix). We can see that the experimental measurements agree well with the theoretical and simulation results. Figure 3(c) depicts the intensity distribution of the magnetic field in the TI nanocavity at the absorption peak wavelength. It shows that the magnetic field is confined and distinctly enhanced in the nanocavity. As shown in Fig. 2(d), there are large extinction coefficients for the TI at near-infrared wavelengths, which means that the TI nanocavity possesses high optical loss. Thus, the Fabry–Perot resonance in the asymmetric cavity can give rise to relatively strong light absorption in the near-infrared region.13 The absorption ratio between the TI and silver nanofilms is , revealing that the light absorption mainly stems from the TI nanofilm [see Fig. S8(a) in the Supplementary Material]. From Fig. S8(b) in the Supplementary Material, we can see that the TI bulk dominates in the light absorption of nanofilm, and the surface layers induce a slight redshift of the resonance absorption peak. Moreover, we deposited a 30-nm silver film on the photonic crystal and measured the spectral response (see Fig. S9 in the Supplementary Material). The result demonstrates that there exists a narrow reflection dip and an absorption peak at the wavelength of , which results from the formation of Tamm plasmons in the silver/photonic crystal multilayer. Both the and silver/photonic crystal structures present relatively strong light absorption at the wavelengths from 1545 to 1580 nm. Intuitively, the TI nanocavity/photonic crystal structure would present stronger absorption at these wavelengths, but a distinct transparency window appears around 1550 nm in the absorption spectrum, as shown in Fig. 1(f). The generation of reflection dips in the silver/photonic crystal structure is similar to the Tamm plasmon response in previous structures.49
Figure 3.TI thickness-dependent nanocavity resonance and induced transparency. (a) Experimentally measured absorption spectra of the TI nanocavities on the
Figure 4.EIT-like response with different silver film thicknesses. (a) Theoretical evolution of absorption spectrum from the TI nanocavity/photonic crystal structures with different silver film thicknesses
As depicted in Fig. 4(b), the experimental results verify the theoretical prediction of spectral evolution. To clarify the mechanism of the EIT-like effect, we theoretically fitted the measured absorption spectra with the two-coupled-oscillator (TCO) model (see Appendix). The results show that the decaying rate of oscillator 1 (TI nanocavity) slightly changes as the TI thickness varies from 15 to 50 nm. is when . The decaying rate of oscillator 2 (silver/photonic crystal structure) slowly increases with and can approach when . The coupling strength between oscillators 1 and 2 rapidly decreases as increases. reaches when , which is much less than the threshold coupling strength []. Therefore, the coupling between the nanocavity resonance and Tamm plasmons is located in the weak-driving regime when .29 The coupling phase retardation approaches in the TI nanocavity/photonic crystal structures with different (see Fig. S10 in the Supplementary Material), verifying the destructive interference between the nanocavity resonance and Tamm plasmons. Because the coupling strength satisfies the criterion , the observed transparency windows in our systems are attributed to the EIT-like effect with the existence of large and small even when declines to 15 nm, as depicted in Fig. 4(c). Thus, the EIT-like response can be achieved in the TI nanocavity/photonic crystal structure with a film thickness of . The absorption dip can approach a low value of 6% at the 1550-nm wavelength when (see Fig. S11 in the Supplementary Material). It means that the EIT-like effect can effectively bypass the optical loss in the structure with a small silver thickness.
3 Discussion
The TI possesses an ultrahigh refractive index at near-infrared wavelengths, much exceeding the conventional HRI Si and Ge semiconductors [see Fig. 2(d)]. The ultrahigh refractive index of TI enables the realization of planar cavities with tens of nanometers in thickness, which can find promising applications in light–matter interaction, for instance, infrared optoelectronic conversion. From Fig. 1(c) and Fig. S3 in the Supplementary Material, we can see that the TI cavity with a 42-nm film presents an ultrabroad resonance absorption of light with high efficiency of at the wavelengths from 970 to 1850 nm. The nanocavities can effectively break the absorption limit of 50% for ultrathin free-standing film at near-infrared range.55 As shown in Fig. S8 in the Supplementary Material, the light absorption mainly stems from the TI nanofilm with a narrow-bandgap semiconducting property. The absorption ratio between the TI and silver nanofilms is around the resonance wavelength. The TI cavities will contribute to the high-efficiency, broad-spectrum, ultrathin, and large-area near-infrared optoelectronic devices, e.g., telecommunication band photodetectors.
From Fig. 3(b), we can see that the resonance wavelength presents a linear redshift with the increasing TI thickness. The resonance wavelength is times as large as the TI nanocavity thickness (), which is more remarkable than the subwavelength-thin () layer of Ge nanostructures.55 This property also enables the precision monitoring of nanofilm thickness in the deposition process.13 To achieve this kind of optical cavities, the thicknesses of TI are much thinner than those of HRI Si and Ge semiconductors (see Fig. S12 in the Supplementary Material). For example, the TI thickness is (64%) of Si (Ge) thickness for optical resonance at the 1550-nm wavelength. Thus, the thickness of the TI cavity can be improved by 34% (24.5%) compared with that of the Si (Ge) cavity. Moreover, the nanocavities may find applications in ultrathin structures for wavefront shaping, similar to Si metasurfaces.8
The TI nanocavities will offer new building blocks for realizing novel optical effects. Herein, we have innovatively integrated the TI nanocavity onto a photonic crystal with alternately stacked and layers. Interestingly, an analogy to the atomic EIT effect has been observed at telecommunication wavelengths. This EIT-like behavior is attributed to the destructive interference coupling between the resonance in TI nanocavity and Tamm plasmons in silver/photonic crystal structure. Compared with the conventional materials, the TI with relatively high refractive index and extinction coefficient has the specific advantage for the generation of the EIT-like effect in this system (see Fig. S13 in the Supplementary Material). Besides the nanocavity thicknesses, the EIT-like response is also dependent on the incident light angle. From Fig. S14 in the Supplementary Material, we can see that the induced transparency wavelength exhibits a blueshift with the increase of incident light angle. This stems from the identical shift of the Tamm plasmon wavelength by altering the incident light angle. The shifted wavelength of s-polarized light is different from that of p-polarized light, which stems from the energy splitting between the s- and p-polarized Tamm states.49 The adjustment of the incident light angle offers an effective way for dynamic tunability of the induced transparency window. The induced transparency spectrum can also be tuned by controlling the polarization of light at oblique incidence, as shown in Fig. S14(f) in the Supplementary Material. This kind of cavity structures based on planar multilayers can effectively avoid the fabrication process and area limitations of the structures based on dielectric or metallic nanoparticles for the generation of EIT-like effects. The EIT-like effect presents good robustness to the alteration of the environmental refractive index (see Fig. S15 in the Supplementary Material). The TI nanocavity also enables the formation of EIT-like behavior by integrating with the thin Ge and silver layers (see Fig. S16 in the Supplementary Material). The thickness can be effectively improved when compared with the Ge-based cavity. This work will open a new door for ultrathin optical cavities and promote the applications of TIs in light control and optical functional devices.
4 Appendix: Methods
4.1 Fabrication
The TI and silver nanofilms were prepared by the MS deposition technique. The film was deposited using radio-frequency (RF) sputtering with a pressure of 0.9 Pa and power of 70 W. The silver film was deposited using the direct current sputtering with a pressure of 0.6 Pa and power of 50 W. The feasible grown area can be set as for the flat nanofilms in our MS deposition. The 2-nm layer was deposited by employing the RF sputtering with a pressure of 1 Pa and power of 100 W. The flowing Ar (100 sccm) was employed as the sputtering gas. The 1D photonic crystal with alternately stacked and layers was prepared on the polished substrate (Beijing Dream Material Technology Co., Ltd.) through electron beam deposition.
4.2 Characterizations and Measurements
The surface flatness of grown TI nanofilm was characterized using the commercial SEM equipment (FEI Verios G4) and AFM system (Bruker Dimension FastScan). The AFM system was also used to test the thicknesses of deposited films. The material morphology of TI nanofilm was characterized through the SAED pattern and HRTEM image, which were measured using the TEM equipment (FEI Talos F200X) with a voltage of 200 kV. The Raman spectrum of TI was measured using a confocal microspectrometer (WITec Alpha300R) with a 532-nm laser. The complex refractive index of TI in the optical region was tested by employing a spectroscopic ellipsometer (HORIBA UVISEL Plus) with a 70-deg incident light angle. The absorption, reflection, and transmission spectra of fabricated samples were measured using a spectrophotometer (Hitachi UH5700).
4.3 Simulations
To verify the experimental results, we employed the FDTD method to numerically simulate the optical spectra and field distributions of TI nanocavity and TI nanocavity/photonic crystal structures.56 In FDTD simulations, the bottom and top of structures were set as the perfectly matched layer absorbing boundary conditions. The other sides of computational space were set as the periodic boundary conditions. The non-uniform mesh was utilized in the -axis direction to fully consider the influence of each layer. The mesh size of the TI surface layer was set as 0.3 nm. The maximum mesh size of other layers was 5 nm. The absorption spectra of the entire structures were achieved with , where , , and denote the powers of reflected, transmitted, and incident light, respectively. The complex refractive indices of TI surface and bulk were set as the measured values in Figs. 2(e) and 2(f). The measured complex refractive index of MS-deposited silver film was used in the simulations (see Fig. S7 in the Supplementary Material). The refractive indices of and were set as 1.44 and 2.058 at the wavelengths of interest, respectively.57,58 The refractive indices of Si and Ge in the simulations come from the experimental data.59,60
4.4 Theory
To clarify the mechanism of the EIT-like effect in the TI nanocavity/photonic crystal structures, we theoretically studied the EIT-like spectra with the TCO model.31,53 As shown in Fig. 1(c), the resonant mode in the TI nanocavity (i.e., oscillator 1) can be generated when the light is incident on the TI nanofilm. Tamm plasmons in silver/photonic crystal structure (i.e., oscillator 2) can be excited by the resonant coupling of TI nanocavity. As depicted in the inset of Fig. 1(f), stands for the resonant frequency of oscillator 1. is the frequency detuning between oscillators 1 and 2. and are the decaying rates of oscillators 1 and 2, respectively. is the complex coupling coefficient between the two oscillators with a coupling phase retardation . When , , and , the light absorption in the entire structure can be described as
Hua Lu is as a professor at Northwestern Polytechnical University in China. He received his PhD from the Chinese Academy of Sciences. He was a postdoc fellow at Swinburne University of Technology in Australia, and then joined Northwestern Polytechnical University in 2015. His current research interest is focused on nanophotonics, plasmonics, and nanomaterials. To date, he has published more than 100 articles in professional journals, including Light Sci. Appl., Adv. Photon., Laser Photon. Rev., and Small, with citation counts of
Jianlin Zhao is a chief scientist at Northwestern Polytechnical University and the director of MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions. He has been selected as a fellow of the Chinese Optical Society and the executive editor-in-chief of Acta Optica Sinica. His research interests include micro-/nanophotonics, light-field manipulation, digital holography, and optical fiber sensing. To date, he has published three textbooks (sole author) and more than 500 articles in professional journals, including Science, Nat. Mater., Adv. Mater., Light Sci. Appl., and Nat. Commun., with citation counts of >13,000. He was continuously selected as Elsevier’s Highly Cited Chinese Researcher (2021–2023).
Biographies of the other authors are not available.
[18] H. Krishnamoorthy et al. Topological insulator metamaterials. Chem. Rev., 123, 4416-4442(2023).
[21] H. Lu, P. Yu, H. Xu, Z. Wang et al. Topological insulator plasmonics and enhanced light-matter interactions. Plasmon-Enhanced Light-Matter Interactions, 89-116(2022).
[56] A. Taflove, S. Hagness. Computational Electrodynamics: The Finite-Difference Time-Domain Method(2000).
[59] E. Palik. Handbook of Optical Constants of Solids(1998).
[60] M. J. Weber. Handbook of Optical materials(2003).
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Hua Lu, Shouhao Shi, Dikun Li, Shuwen Bo, Jianxu Zhao, Dong Mao, Jianlin Zhao, "
Category: Research Articles
Received: Oct. 27, 2023
Accepted: Mar. 14, 2024
Published Online: Apr. 7, 2024
The Author Email: Lu Hua (hualu@nwpu.edu.cn), Zhao Jianlin (jlzhao@nwpu.edu.cn)