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[Ming‐Jyun Ye](https://orcid.org/0000-0003-2307-1461), Rashid G. Bikbaev, Pavel S. Pankin, Lu‐Hsing Chen, David Chiu, Ivan V. Timofeev, Hung‐Wen Chen, [Satoshi Ishii](https://orcid.org/0000-0003-0731-8428), Kuo‐Ping Chen

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This is the peer reviewed version of the following article: M.-J. Ye, R. G. Bikbaev, P. S. Pankin, L.-H. Chen, D. Chiu, I. V. Timofeev, H.-W. Chen, S. Ishii, K.-P. Chen, Lossless Phase Change Materials for Adjustable Tamm Plasmon Polaritons in the Near-Infrared. Adv. Optical Mater. 2025, 13, 2402889, which has been published in final form at https://doi.org/10.1002/adom.202402889. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.[In Copyright](http://rightsstatements.org/vocab/InC/1.0/)

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[Lossless Phase Change Materials for Adjustable Tamm Plasmon Polaritons in the Near‐Infrared](https://mdr.nims.go.jp/datasets/ea097c30-2006-4279-9de3-5699b783a8a0)

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Template for Electronic Submission to ACS JournalsLossless Phase Change Materials for Adjustable Tamm Plasmon Polaritons in the Near-infrared  Ming-Jyun Ye 1,2, Rashid G. Bikbaev 3,4, Pavel S. Pankin3,4, Lu-Hsing Chen3, David Chiu6,  Ivan V. Timofeev 3,4, Hung-Wen Chen 3, Satoshi Ishii 2, and Kuo-Ping Chen 3 *  1 College of Photonics, National Yang Ming Chiao Tung University, Tainan, Taiwan 2Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), Tsukuba, Japan 3 Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, Taiwan 3Kirensky Institute of Physics, Federal Research Center KSC SB RAS, Krasnoyarsk 660036, Russia 4 Institute of Engineering Physics and Radio electronics, Siberian Federal University, Krasnoyarsk 660041, Russia 6International Intercollegiate Ph.D. Program, National Tsing Hua University, Hsinchu 300044, Taiwan *kpchen@ee.nthu.edu.tw  *Corresponding Author: kpchen@ee.nthu.edu.tw ABSTRACT: Incorporating a phase-change materials (PCM) to a nanophotonic structure is a straightforward way to make it tunable. The binary semiconducting chalcogenide, antimony trisulfide (Sb2S3), is a suitable PCM for nanophotonic applications in the near-infrared (NIR) owing to its high refractive index, low optical losses, and wide bandgap properties. Here, the Sb2S3 layer is embedded between the distributed Bragg reflector (DBR) and the metal layer where Tamm plasmon polaritons (TPPs) are excited at the interface. The TPP resonance shift of 45 nm is caused by the phase change of Sb2S3 from amorphous to crystal. Also, the resonance shifts of 85 nm, 76 nm, and 63 nm are achieved by unpolarized, TM mode, and TE mode NIR light, respectively, depending on oblique angle incidences. KEYWORDS: Antimony trisulfide, distributed Bragg reflector, phase-change materials, Tamm plasmon polaritons metasur-face, high refractive index Introduction  Optical communication has received great attentions in the recent years. Silicon and germanium photonics have been com-patible with complementary metal-oxide semiconductor (CMOS) technology in photonic integrated circuits (PICs)1 2, 3. Variety of PIC elements have developed to manipulate light through optical couplers3, 4, modulators5, 6, polarization beam splitters7, 8, and optical filters9, 10. Based on passive and active PIC designs, versatile elements have been developed in different areas such as flash memory11, quantum information12, 13, biosensor14, 15, and electric vehicle16. They were called application-specific pho-tonic integrated circuits (ASPICs)17. For the development of nanophotonics devices, plasmonics and metasurfaces are the two emerging research fields. How-ever, as they typically involve complex 2D and 3D nanostructure, it is challenging for large area fabrication 18, 19. Among the nanophotonic designs, even with a one-dimensional (1D) planar photonic, obtaining high-Q resonance is possible, known as Tamm plasmon states. The Tamm plasmonic state is one of the photonic resonances experimentally demonstrated between the distributed Bragg reflector (DBR) and a metal layer, which excites Tamm plasmon polaritons (TPPs) 20, 21. It has electric-field solid confinement at the interface, high design wavelength resolution, and independent incidence polarization compared to surface plasmon polaritons. When researchers further explored tunable TPP devices, liquid crystals were considered to enable switchable functionality in TPP systems22 . Even though liquid crystals are matured materials, they still have some problems with modulation speed and static power consumption in LiDAR systems or micro-scale liquid-crystal-based device23. There-fore, this paper proposes a nonvolatile-reconfigurable solid-state 1D nanophotonic sensor that can tune the TPP resonances in the near-infrared.  In addition to liquid crystals, phase-change materials (PCMs) have been widely applied in switchable electronics and pho-tonics 24-28. Typically used PCMs include vanadium dioxide (VO2), germanium-antimony-tellurium (GST), and antimony tri-sulfide (Sb2S3). The crystal phase of VO2 was switched from a monoclinic state near 340 K. The working system of GST was above 380 K at the communication wavelength.  Moreover, these two PCMs have a high extinction coefficient of around 0.5 and 2.0 in the visible, respectively 29. On the Contrary, a binary semiconducting chalcogenide Sb2S3 has a band gap of 1.8 to 2.1 eV such that the absorption band edge is in the visible. Meanwhile, the high refractive index (HRI) of Sb2S3 can be tuned from 3 to 4 at around 650 nm. Also, its extinction coefficient was below 0.05 longer than 700 nm in both states. The nonvolatile property of Sb2S3 decreases the energy consumed to keep it in its original state that satisfies the green and environmentally friendly. Therefore, Sb2S3 has been a good candidate for nanophotonic design in the NIR spectrum. Sreekanth reported that Sb2S3 and SiO2 acted as pair layers of DBR to achieve the TPP signal for surface-enhanced Raman spectroscopy (SERS)30. However, we found that such an HRI refractive material was sensitive when combined with DBR. In other words, it was not easy to control the same Sb2S3 thickness in each pair due to its high evaporate rate, leading to unexpected wavelength variations. Therefore, in this investigation, Sb2S3 was used as a reconfigurable functional layer in the PC-TPP structure. After the anneal-ing process, the modulable wavelength was demonstrated to be around 45 nm. In addition, the three types of PCM were dis-cussed with the same sub-wavelength thickness in the PC-TPP simulation design. Moreover, the analysis of angle-dependent resonance was also proved to be about 85 nm from in NIR. It was shown that our design would support in LiDAR 31, 32, and sensor 33 applications. mailto:*kpchen@ee.nthu.edu.tw 2  RESULTS AND DISCUSSION The optical constant of three phase change materials (Sb2S3, VO2, and GST) were shown in Figure 1. See Figure 1 (a); as grown, Sb2S3 (blue line) was deposited by evaporation and turned polycrystalline (red line) via annealing. See blue dash line; the absorption coefficient (above 600 nm) was like Si3N4, which has been widely used for all-dielectric metasurface in the visible spectrum for filter34, 35, lasing cavity36. After the phase change, shown as the red dashed line, the absorption coefficient of c-Sb2S3 was also lossless above 700 nm. In Figure 1 (b), VO2 was fabricated via sputter and underwent annealing. In addition, it was captured to tune the phase change property through a low phase change temperature. Such dynamic material has been used in smart windows37, 38, sensor39, cloak technology40 and memristor41. However, it was unsuitable to design as all-VO2 metasurface because of its high optical loss in the visible. Figure 1 (c) plots the optical constant of GST, which is taken from the reference42. GST have been often used in MIR as they have large absorption coefficients in visible wavelengths.  Figure 1. Optical constants of (a) Sb2S3 (b) VO2, and (c) GST42. Phase change materials, including Sb2S3, VO2, and GST, in the form of TPP devices, are discussed in Figure 2. VO2 and GST have been exploited in photonic devices over 1.5 m due to their intrinsic material loss in the visible spectrum. Although they were suggested near 1.1 m, they were only used as a functional ultrathin layer43-45. Moreover, they were driven with DBR design in communication wavelength, and the thickness of DBR was thicker, which was inappropriate for modern quan-tum or optical devices. Therefore, Sb2S3 is suitable for reconfigurable designs in the metasurface or TPP in the NIR spectrum due to its lossless and large bandgap shift25, 46. The finite-difference time-domain (FDTD) method was used to calculate the phase change Tamm plasmon–polaritons (PC-TPP) resonance with normal light incidence at 600 nm to 1100 nm. In this mod-eling, the DBR has eight pairs of 145 nm silica and 95 nm TiO2. The reflectance spectrum showing the DBR stop band is shown in grey area in Figure 2. In Figure 2 (a) and 2(b), the blue and red lines are the reflectance spectra of a- and c- Sb2S3 TPP, respectively, where the resonance wavelength shifted from 886 nm to 959 nm after the phase change process, resulting in a wavelength shift of 73 nm. Additionally, the mode characterization of shorter 741 nm resonance was discussed in Figure S7. In the modeling, the phase-change-material layer in each TPP case was set at the same thickness, 144 nm, with a 30-nm thick gold. It can be seen from Figure 2 (c) that conjugated the s-VO2 with a metal layer, and PhC leads to low Q-factor TPP. Phase transition of the VO2 from semiconductor to metal state leads to changing the phase matching condition for the TPP. As a result, the TPP wavelength shifts beyond the PhC band gap. In Figure 2 (d), the a- and c- GST (dark-brown and brown line, respectively) had no resonance dips.   3  Figure 2. (a) Schematic of the TPP structure. Numerically simulated reflectance spectra of the Au-PCM-PhC structure with 144 nm PCM thickness for (b) a- and c-Sb2S3 TPP, (c) s- and m- VO2 TPP, and (d) a- and c-GST TPP in the NIR.  The thickness-dependent spectrum of Sb2S3 TPP was simulated in Figure 3. In Figure 3 (a), the a-Sb2S3 TPP resonance was approximately 740 nm while c-Sb2S3 was around 780 nm with a thickness of 50 nm. As this thickness was greater than 150 nm, the TPP resonance of the amorphous and crystalline phases red-shifted, and they were at around 930 nm and 990 nm, respectively. At around 700 nm, the unexpected resonance was near the band edge of the DBR. In Figure 3(b), s-VO2 and m-VO2 TPP do not have a noticeable dip in the specific spectrum. In Figure 3 (c), neither had a clear resonance in the GST TPP case. Overall, compared to VO2 and GST, Sb2S3 is a better candidate for manipulating the desired resonance with TPP in the NIR spectrum. Furthermore, it showed good development potential in the LiDAR area.  The dependence of the TPP wavelength on the PCM film thickness could be calculated analytically by solving the dis-persion relations of TPP. A detailed description of the procedure for deriving the dispersion law for TPP was provided in the Supplementary Material. In general, the solution to the dispersion relations is a complex frequency. The real part of this com-plex frequency corresponds to the TPP wavelength inside the PhC band gap, while the imaginary part corresponds to the spectral width of the resonance line. The calculated real part of the complex frequency was presented in Figure 3 (a) in small circles. The results obtained by the TCMT and FDTD methods agree reasonably well. A slight difference near the edge of the PhC band gap was caused by the dispersion equation derived for a metal film combined with a semi-infinite PhC. In contrast, in the experiment, the number of the PhC periods was eight.  4  Figure 3. Simulated thickness-dependent spectra of Au-PC-PhC structures with (a) Sb2S3, (b) VO2, and (c) GST as PCMs.  The optical bandgap was derived with the direct bandgap calculation through the Tauc equation by measuring the reflectance and transmittance of the films deposited on glass substrates. As shown in Figure 4 (a), the bandgap of a-Sb2S3 was 2.14 eV, and the curve feature shows a direct bandgap. In Figure 4 (b), the bandgap of c-Sb2S3 was shifted to 1.85 eV after the phase change process. Figures 4 (c) and (d) present the Raman spectra of the a- and c-Sb2S3, respectively. In the case of c-Sb2S3 case, the two major peaks, 282 and 301 cm-1, correspond to the antisymmetric S-Sb-S stretching modes, and 147 cm-1 corresponds to the Sb metallic phase25, 47, 48.   Figure 4. Tauc plots for (a) a-Sb2S3 and (b) c-Sb2S3. Optical bandgap energies were calculated with the Tauc function by measuring the reflectance and Transmittance of Sb2S3 on a glass. The Raman spectrum of (c) a-Sb2S3 and (d) c-Sb2S3. While a-Sb2S3 shows a broad bandwidth, c-Sb2S3 has two major peaks at 282 and 301 cm-1. The metallic phase of Sb appears at 147 cm-1. Figure 5(a) shows the cross-section SEM image of the Sb2S3 TPP sample where periodic DBR multilayers are clearly shown. The experimental results of the Sb2S3 TPP sample achieved 45 nm wavelength shift from 886 nm to 932 nm after annealing the sample from amorphous (blue solid line) to crystal state (red solid line), as shown in Figure 5 (b). The experiment and simulation results were different because the annealing process could have resulted in the decrease of Sb2S3 films. The first reason was that the density of amorphous was 26% less than crystalline49. Secondly, we tested the annealing process in  5 the atmosphere and vacuum, resulting in oxidation and thinning, respectively. Hence, the Sb2S3 could be deposited with a few transparent dielectric layers (Al2O3 or Si3N4) to protect it within the phase change process in some research on the fabrication of the Sb2S3 metasurface25, 46, 50. In our Sb2S3 TPP case, the film thickness decreased around 30 nm after annealing. To avoid the thickness decrease of Sb2S3, the gold film was first deposited on a- Sb2S3 to maintain 128 nm c- Sb2S3 after the annealing.  The electric displacement field of the photonic device is shown in Figure 5 (c), and the most robust confinement was between Sb2S3 and gold film. In Figure 5 (d), the extensive refractive index modulation at the Sb2S3 shows that it has the HRI property compared to silicon in the NIR.  Figure 5. The experimental and E-field result of Sb2S3 TPP device. (a) SEM image. The SiO2 and TiO2 are shown in white and brown ar-rows, respectively.  (b) The TPP resonance shifted from 886 nm to 932 by the phase change. (c) The electric field intensity profile of fun-damental TPP mode with the incident light from air. (d) The refractive index profiles when the Sb2S3 is in amorphous and crystal phases.   In Figure 6 (a), angle-dependent reflectance was measured from 16o to 60o in the a-Sb2S3 PC-TPP case with a homemade system aiming for LiDAR application.  The TPP resonance has a wavelength shift of 85 nm from 878 to 793 nm. The TPP resonance displayed a blue-shifted and slightly enhancing reflectance at larger oblique angles. It is con-sistent with the references that they theoretically computed transverse electric (TE) and transverse magnetic (TM) prop-erties51, 52. However, while the wavelength variation of the experimental result fits well with the simulation, shown in Figure 6, we found that the dip was divided into two as the angles increased and started from 40º, the results were collected without a polarizer.  After the incident light was set as TE and TM mode, the results were manipulated by a-Sb2S3 TPP (details were shown in the Supplementary Information Figure S2). In TM mode, the reflectance results were kept within 8~12%, and the wavelength was from 873 nm to 797 nm (~76 nm shifted), while the angles were from 22o to 58o. In TE mode, the reflectance results changed from 13% to 40% when the wavelength was changed from 873 nm to 810 nm (~63 nm shifted). TE and TM were aligned through the same oblique angles with a starting wavelength of 873 nm, and the reflec-tance was almost the same at 12~13%. They had gradual varieties after the oblique angle was above 40o (847 nm). Meanwhile, the TM mode was moved to the blue-shift wavelength of 13 nm more than the TE mode. Furthermore, the spectrum of Figure S2 (c) derived from Figures S2 (a) and S2 (b) agreed with the trend of Figure 6. Hence, these results provided a new path for selective wavelength or intensity of signal applications in TE, TM, or unpolarized cases.  The c-Sb2S3 TPP device was also discussed in the Supplementary Information Figure S4. The results measured with an unpolarized light source also showed blue-shift and split peaks at large oblique angles. However, the reflectance and quality factor did not fit enough. The reason was that part of the Sb2S3 film on the last layer of DBR partially peeled off after the annealing progress of c-Sb2S3 TPP, which others hardly mentioned earlier. Hence, the Sb2S3 could be deposited with a few transparent dielectric layers (Al2O3 or Si3N4) to protect it within the phase change process in some research on the fabrication of the Sb2S3 metasurface25, 46, 50.   6  Figure 6. Un-polarized angle-dependent spectrum of a-Sb2S3 PC-TPP device (a) experiment and (b) simulation. (y-axis: max 100%, min 0%)  CONCLUSIONS In conclusion, our work has shown that the lossless, high refractive index, and large refractive contrast properties of Sb2S3 are promising for versatile applications in NIR compared to other PCMs. With the current TPP design, the thick-ness of the Sb2S3 can be designed within this DBR stopband from 750 to 1000 nm. In the experiment, after phase transi-tion, the resonance shift of 45 nm was demonstrated for the of Sb2S3 TPP from 886 nm to 932 nm. The main advantage of adopting Sb2S3 in this work, compared to other PCMs like VO2 and GST, is an ultra-low extinction coefficient (~ 0) above 700 nm in both amorphous and crystalline states. This low optical loss ensures minimal energy dissipation and high-quality resonance in the visible to near-infrared (NIR) spectrum. In addition, the angle-dependent spectrum was systematically discussed in unpolarized, TE, and TM modes in simulation and experiment from 16o to 60o. The a-Sb2S3 PC-TPP resonance has a significant wavelength shift of 85 nm (from 878 to 793 nm). This is the largest wavelength modulation in TPP devices reported so far. For the returning process from crystalline to amorphous state, it could be realized by femto-second laser25 or electrical short pulse quenching46. However, damaging the metal films should be avoided. With this regard, the refractory plasmonic materials could be considered53, 54. This research provides an essential guideline for studying high-Q adjustable 1D-photonic with lossless and high refractive index, phase change materials. The potential applications of the work include optical memory, optical data storage, and LiDAR receiver systems. EXPERIMENTAL SECTION To fabricate the Sb2S3 TPP device, the DBR layers (SiO2 and TiO2) were first fabricated via E-beam evaporation. Gold film and Sb2S3 were also deposited on the DBR through E-beam evaporation. The gold/a-Sb2S3/DBR sample was annealed at 250 °C for two hours in a vacuum furnace at a rate of 0.15 °C/sec to become the gold/c-Sb2S3/DBR sample. The refractive index and extinction coefficient were collected by a spectroscopic ellipsometer (J. A. Woollam). Raman spectra were measured by a WITec alpha300 (WITec, GmbH, Germany) with a 532 nm CW laser. The reflectance and transmittance spectra were collected by an optical microscope (BX51, Olympus) with a 20× objective lens (NA = 0.4) and passed through two spectrum sensors (SE2020-025-FUV, SW2540) to cover a wide spectral range. The angle-dependent spectrum was measured by a homemade angle-dependent measurement system.  Corresponding Author *E-mail: kpchen@ee.nthu.edu.tw Notes. The authors declare no competing financial interest. ACKNOWLEDGMENT  This work is supported by the National Science and Technology Council (NSTC; 111-2923-E-007-008-MY3; 111-2628-E-007-021; 112-2223-E-007 -007 -MY3; 112-2923-E-007 -004 -MY2; 112-2119-M-A49-008). This research was also funded by the Russian Science Foundation (project no. 22-42-08003).  7 Uncategorized References 1. Soref, R., Mid-infrared photonics in silicon and germanium. Nature photonics 2010, 4 (8), 495-497. 2. 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