Understanding the Extremely Poor Lattice Thermal Transport in Chalcogenide Perovskite BaZrS₃

Abstract

Combining first-principles calculations with the solution to the Boltzmann transport equations, we examine the lattice thermal transport for the orthorhombic perovskite BaZrS3 through analyses of phonon group velocities, lifetimes, average Grüneisen parameter, and Debye temperature. An extremely low lattice thermal conductivity (LTC) of 1.16 Wm–1 K–1 at 300 K is obtained with phonons at 0–4 THz being the main contributors. The acoustic phonons contribute ∼30% to the LTC, while the lower frequency range of the optical modes contributes the most. Nearly 83% of the accumulated LTC is contributed by phonons with MFP < 5 nm. Since the lattice parameter (9.98 Å) of BaZrS3 is not significantly different from the calculated MFP, we corroborate that nanostructuring might be ineffective to reduce LTC.

Ultralow Lattice Thermal Conductivity at Room Temperature in Cu4TiSe4

“…Cu-based chalcogenide materials (in bulk) have been extensively investigated for the application of thermoelectric [13][14][15][16][17][18][19][20][21][22][23][24] and photo-voltaic [25][26][27][28][29] over the past few years.H igh natural abundance,low cost of Cu and chalcogens (e.g. S, Se) and suitable band gaps have made them very attractive candidates for photovoltaic applications.…”

High frequency atomic tunneling yields ultralow and glass-like thermal conductivity in chalcogenide single crystals

“…Such homogeneous single crystals with low defect concentrations usually exhibit the familiar trend of decreasing thermal conductivity with increasing temperature above the Debye temperature 18 . Within the perovskite material family, the thermal conductivity varies from 1 to 20 W m −1 K −1 for the simplest ABO 3 -type perovskite oxides [19][20][21] and chalcogenides 22 , and <1 W m −1 K −1 for organic-inorganic hybrid perovskites 23 and inorganic halides 24 , although all of these materials follow the crystalline trend of thermal conductivity with temperature.…”

Colloidal BaZrS3 chalcogenide perovskite nanocrystals for thin film device fabrication

“…The thermal expansion coefficient serves as a design parameter for materials having low thermal lattice conductivity, and hence has application in designing thermoelectric materials 47. This low thermal volume expansion of BaZrS 3 NCs gives an indication that they could have low thermal conductivity which has been recently reported 48,49. To study the local structure of BaZrS 3 NCs, we have recorded the temperature-dependent X-ray absorption fine structure (XAFS) data of the samples at the Zr K-edge in the transmission mode at the Scanning EXAFS beamline (BL-09) at the Indus-2 synchrotron source (2.5 GeV, 200 mA) at the Raja Ramanna Centre for Advanced Technology (RRCAT), Indore, India.…”

“…47 This low thermal volume expansion of BaZrS 3 NCs gives an indication that they could have low thermal conductivity which has been recently reported. 48,49 To study the local structure of BaZrS 3 NCs, we have recorded the temperature-dependent X-ray absorption fine structure (XAFS) data of the samples at the Zr K-edge in the transmission mode at the Scanning EXAFS beamline (BL-09) at the Indus-2 synchrotron source (2.5 GeV, 200 mA) at the Raja Ramanna Centre for Advanced Technology (RRCAT), Indore, India. The details of the experimental methodology and data analysis are given in the ESI.…”