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1. Raman study of layered breathing kagome lattice semiconductor Nb ₃ Cl ₈

   https://doi.org/10.1088/2053-1583/acfa10  

   Jeff, Dylan A; Gonzalez, Favian; Harrison, Kamal; Zhao, Yuzhou; Fernando, Tharindu; Regmi, Sabin; Liu, Zhaoyu; Gutierrez, Humberto R; Neupane, Madhab; Yang, Jihui; et al (September 2023, 2D Materials)

   Abstract Niobium chloride (Nb₃Cl₈) is a layered two-dimensional semiconducting material with many exotic properties including a breathing kagome lattice, a topological flat band in its band structure, and a crystal structure that undergoes a structural and magnetic phase transition at temperatures below 90 K. Despite being a remarkable material with fascinating new physics, the understanding of its phonon properties is at its infancy. In this study, we investigate the phonon dynamics of Nb₃Cl₈in bulk and few layer flakes using polarized Raman spectroscopy and density-functional theory (DFT) analysis to determine the material’s vibrational modes, as well as their symmetrical representations and atomic displacements. We experimentally resolved 12 phonon modes, five of which areA_1gmodes while the remaining seven areE_gmodes, which is in strong agreement with our DFT calculation. Layer-dependent results suggest that the Raman peak positions are mostly insensitive to changes in layer thickness, while peak intensity and full width at half maximum are affected. Raman measurements as a function of excitation wavelength (473–785 nm) show a significant increase of the peak intensities when using a 473 nm excitation source, suggesting a near resonant condition. Temperature-dependent Raman experiments carried out above and below the transition temperature did not show any change in the symmetries of the phonon modes, suggesting that the structural phase transition is likely from the high temperatureP $\overline{\text{3}m}$1 phase to the low-temperatureR $\overline{3m}$phase. Magneto-Raman measurements carried out at 140 and 2 K between −2 and 2 T show that the Raman modes are not magnetically coupled. Overall, our study presented here significantly advances the fundamental understanding of layered Nb₃Cl₈material which can be further exploited for future applications. 

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2. Raman spectroscopy of phonon states in NbTe ₄ and TaTe ₄ quasi‐one‐dimensional van der Waals crystals

   https://doi.org/10.1002/jrs.6661  

   Nataj, Zahra_Ebrahim; Kargar, Fariborz; Krylyuk, Sergiy; Debnath, Topojit; Taheri, Maedeh; Ghosh, Subhajit; Zhang, Huairuo; Davydov, Albert_V; Lake, Roger_K; Balandin, Alexander_A (February 2024, Journal of Raman Spectroscopy)

   Abstract We report the results of polarization‐dependent Raman spectroscopy of phonon states in single‐crystalline quasi‐one‐dimensional NbTe₄and TaTe₄van der Waals materials. The measurements were conducted in the wide temperature range from 80 to 560 K. Our results show that although both materials have identical crystal structures and symmetries, there is a drastic difference in the intensity of their Raman spectra. While TaTe₄exhibits well‐defined peaks through the examined wavenumber and temperature ranges, NbTe₄reveals extremely weak Raman signatures. The measured spectral positions of the phonon peaks agree with the phonon band structure calculated using the density‐functional theory. We offer possible reasons for the intensity differences between the two van der Waals materials. Our results provide insights into the phonon properties of NbTe₄and TaTe₄van der Waals materials and indicate the potential of Raman spectroscopy for studying charge‐density‐wave quantum condensate phases. 

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3. Spin–Phonon Interactions and Anharmonic Lattice Dynamics in Fe ₃ GeTe ₂

   https://doi.org/10.1002/apxr.202200089  

   Cai, Qingan; Zhang, Yuemei; Luong, Diana; Tulk, Christopher_A; Fokwa, Boniface_PT; Li, Chen (March 2023, Advanced Physics Research)

   Abstract Raman scattering is performed on Fe₃GeTe₂(FGT) at temperatures from 8 to 300 K and under pressures from the ambient pressure to 9.43 GPa. Temperature‐dependent and pressure‐dependent Raman spectra are reported. The results reveal respective anomalous softening and moderate stiffening of the two Raman active modes as a result of the increase of pressure. The anomalous softening suggests anharmonic phonon dynamics and strong spin–phonon coupling. Pressure‐dependent density functional theory and phonon calculations are conducted and used to study the magnetic properties of FGT and assign the observed Raman modes,and. The calculations proved the strong spin–phonon coupling for themode. In addition, a synergistic interplay of pressure‐induced reduction of spin exchange interactions and spin–orbit coupling effect accounts for the softening of themode as pressure increases. 

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4. Ultralow lattice thermal conductivity of chalcogenide perovskite CaZrSe3 contributes to high thermoelectric figure of merit

   https://doi.org/10.1038/s41524-019-0253-5  

   Osei-Agyemang, Eric; Adu, Challen Enninful; Balasubramanian, Ganesh (December 2019, npj Computational Materials)

   Abstract An emerging chalcogenide perovskite, CaZrSe₃, holds promise for energy conversion applications given its notable optical and electrical properties. However, knowledge of its thermal properties is extremely important, e.g. for potential thermoelectric applications, and has not been previously reported in detail. In this work, we examine and explain the lattice thermal transport mechanisms in CaZrSe₃using density functional theory and Boltzmann transport calculations. We find the mean relaxation time to be extremely short corroborating an enhanced phonon–phonon scattering that annihilates phonon modes, and lowers thermal conductivity. In addition, strong anharmonicity in the perovskite crystal represented by the Grüneisen parameter predictions, and low phonon number density for the acoustic modes, results in the lattice thermal conductivity to be limited to 1.17 W m⁻¹ K⁻¹. The average phonon mean free path in the bulk CaZrSe₃sample (N → ∞) is 138.1 nm and nanostructuring CaZrSe₃sample to ~10 nm diminishes the thermal conductivity to 0.23 W m⁻¹ K⁻¹. We also find that p-type doping yields higher predictions of thermoelectric figure of merit than n-type doping, and values ofZT~0.95–1 are found for hole concentrations in the range 10¹⁶–10¹⁷ cm⁻³and temperature between 600 and 700 K. 

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5. Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet CrI3

   https://doi.org/10.1038/s41467-020-18627-x  

   Jin, Wencan; Kim, Hyun Ho; Ye, Zhipeng; Ye, Gaihua; Rojas, Laura; Luo, Xiangpeng; Yang, Bowen; Yin, Fangzhou; Horng, Jason Shih An; Tian, Shangjie; et al (September 2020, Nature Communications)

   Abstract Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI₃, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm⁻¹. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by ~50% and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI₃. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors. 

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