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  1. Abstract Optical manipulation of coherent phonon frequency in two-dimensional (2D) materials could advance the development of ultrafast phononics in atomic-thin platforms. However, conventional approaches for such control are limited to doping, strain, structural or thermal engineering. Here, we report the experimental observation of strong laser-polarization control of coherent phonon frequency through time-resolved pump-probe spectroscopic study of van der Waals (vdW) materials Fe 3 GeTe 2 . When the polarization of the pumping laser with tilted incidence is swept between in-plane and out-of-plane orientations, the frequencies of excited phonons can be monotonically tuned by as large as 3% (~100 GHz). Our first-principles calculations suggest the strong planar and vertical inter-atomic interaction asymmetry in layered materials accounts for the observed polarization-dependent phonon frequencies, as in-plane/out-of-plane polarization modifies the restoring force of the lattice vibration differently. Our work provides insightful understanding of the coherent phonon dynamics in layered vdW materials and opens up new avenues to optically manipulating coherent phonons.
    Free, publicly-accessible full text available December 1, 2023
  2. Free, publicly-accessible full text available July 25, 2023
  3. Free, publicly-accessible full text available March 9, 2023
  4. Phonon-mediated thermal transport is inherently multi-scale. The wave-length of phonons (considering phonons as waves) is typically at the nanometer scale; the typical size of a phonon wave energy packet is tens of nanometers, while the phonon mean free path (MFP) can be as long as microns. At different length scales, the phonons will interact with structures of different feature sizes, which can be as small as 0D defects (point defects), short to medium range linear defects (dislocations), medium to large range 2D planar defects (stacking faults and twin boundaries), and large scale 3D defects (voids, inclusions, and various microstructures). The nature of multi-scale thermal transport is that there are different heat transfer physics across different length scales and in the meantime the physics crossing the different scales is interdependent and coupled. Since phonon behavior is usually mode dependent, thermal transport in materials with a combined micro-/nano-structure complexity becomes complicated, making modeling this kind of transport process very challenging. In this perspective, we first summarize the advantages and disadvantages of computational methods for mono-scale heat transfer and the state-of-the-art multi-scale thermal transport modeling. We then discuss a few important aspects of the future development of multi-scale modeling, in particular with themore »aid of modern machine learning and uncertainty quantification techniques. As more sophisticated theoretical and computational methods continue to advance thermal transport predictions, novel heat transfer physics and thermally functional materials will be discovered for the pertaining energy systems and technologies.« less
  5. Thermal anisotropy/isotropy is one of the fundamental thermal transport properties of materials and plays a critical role in a wide range of practical applications. Manipulation of anisotropic to isotropic thermal transport or vice versa is in increasing demand. However, almost all the existing approaches for tuning anisotropy or isotropy focus on structure engineering or materials processing, which is time and cost consuming and irreversible, while little progress has been made with an intact, robust, and reversible method. Motivated by the inherent relationship between interatomic interaction mediated phonon transport and electronic charges, we comprehensively investigate the effect of external electric field on thermal transport in two-dimensional (2D) borophene by performing first-principles calculations along with the phonon Boltzmann transport equation. Under external electric field, the lattice thermal conductivity of borophene in both in-plane directions first increases significantly to peak values with the maximum augmentation factor of 2.82, and the intrinsic anisotropy (the ratio of thermal conductivity along two in-plane directions) is boosted to the highest value of 2.13. After that, thermal conductivities drop down steeply and anisotropy exhibits oscillating decay. With the electric field increasing to 0.4 V Å −1 , the thermal conductivity is dramatically suppressed to 1/40 of the originalmore »value at no electric field. More interestingly, the anisotropy of the thermal conductivity decreases to the minimum value of 1.25, showing almost isotropic thermal transport. Such abnormal anisotropic to isotropic thermal transport transition stems from the large enhancement and suppression of phonon lifetime at moderate and high strength of electric field, respectively, and acts as an amplifying or reducing factor to the thermal conductivity. We further explain the tunability of phonon lifetime of the dominant acoustic mode by an electron localization function. By comparing the electric field-modulated thermal conductivity of borophene with the dielectric constant, it is found that the screened potential resulting from the redistributed charge density leads to phonon renormalization and the modulation of phonon anharmonicity and anisotropy through electric field. Our study paves the way for robust tuning of anisotropy of phonon transport in materials by applying intact, robust, and reversible external electric field without altering their atomic structure and would have a significant impact on emerging applications, such as thermal management of nanoelectronics and thermoelectric energy conversion.« less
  6. A new self-activated X-ray scintillator, BaWO 2 F 4 , with an excellent photoluminescence quantum efficiency is reported. Hydrothermally grown single crystals, space group P 2/ n , exhibit a 3D framework structure containing isolated WO 2 F 4 octahedra. BaWO 2 F 4 exhibits green emission under UV light with a high quantum yield of 53% and scintillates when exposed to X-rays(Cu).