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1. Perspectives on interfacial thermal resistance of 2D materials: Raman characterization and underlying physics

   https://doi.org/10.1007/s44251-024-00037-6  

   Liu, Jing; Al Keyyam, Ibrahim; Xie, Yangsu; Wang, Xinwei (February 2024, Surface Science and Technology)

   Abstract Interfacial thermal resistance plays a crucial role in efficient heat dissipation in modern electronic devices. It is critical to understand the interfacial thermal transport from both experiments and underlying physics. This review is focused on the transient opto-thermal Raman-based techniques for measuring the interfacial thermal resistance between 2D materials and substrate. This transient idea eliminates the use of laser absorption and absolute temperature rise data, therefore provides some of the highest level measurement accuracy and physics understanding. Physical concepts and perspectives are given for the time-domain differential Raman (TD-Raman), frequency-resolved Raman (FR-Raman), energy transport state-resolved Raman (ET-Raman), frequency domain ET-Raman (FET-Raman), as well as laser flash Raman and dual-wavelength laser flash Raman techniques. The thermal nonequilibrium between optical and acoustic phonons, as well as hot carrier diffusion must be considered for extremely small domain characterization of interfacial thermal resistance. To have a better understanding of phonon transport across material interfaces, we introduce a new concept termed effective interface energy transmission velocity. It is very striking that many reported interfaces have an almost constant energy transmission velocity over a wide temperature range. This physics consideration is inspired by the thermal reffusivity theory, which is effective for analyzing structure-phonon scattering. We expect the effective interface energy transmission velocity to give an intrinsic picture of the transmission of energy carriers, unaltered by the influence of their capacity to carry heat. 

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2. Critical problems faced in Raman-based energy transport characterization of nanomaterials

   https://doi.org/10.1039/d2cp02126a  

   Wang, Ridong; Hunter, Nicholas; Zobeiri, Hamidreza; Xu, Shen; Wang, Xinwei (September 2022, Physical Chemistry Chemical Physics)

   In the last two decades, tremendous research has been conducted on the discovery, design and synthesis, characterization, and applications of two-dimensional (2D) materials. Thermal conductivity and interface thermal conductance/resistance of 2D materials are two critical properties in their applications. Raman spectroscopy, which measures the inelastic scattering of photons by optical phonons, can distinct a 2D material's temperature from its surrounding materials', featuring unprecedented spatial resolution (down to the atomic level). Raman-based thermometry has been used tremendously for characterizing the thermal conductivity of 2D materials (suspended or supported) and interface thermal conductance/resistance. Very large data deviations have been observed in literature, partly due to physical phenomena and factors not considered in measurements. Here, we provide a critical review, analysis, and perspectives about a broad spectrum of physical problems faced in Raman-based thermal characterization of 2D materials, namely interface separation, localized stress due to thermal expansion mismatch, optical interference, conjugated phonon, and hot carrier transport, optical–acoustic phonon thermal nonequilibrium, and radiative electron–hole recombination in monolayer 2D materials. Neglect of these problems will lead to a physically unreasonable understanding of phonon transport and interface energy coupling. In-depth discussions are also provided on the energy transport state-resolved Raman (ET-Raman) technique to overcome these problems and on future research challenges and needs. 

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3. Thermophysical properties of 1D materials: transient characterization down to atomic level

   https://doi.org/10.52396/JUSTC-2023-0098  

   Karamati, Amin; Xu, Shen; Lin, Huan; Rahbar, Mahya; Wang, Xinwei (January 2023, JUSTC)

   The thermophysical properties of 1D micro/nanoscale materials could differ significantly from those of their bulk counterparts due to intensive energy carrier scattering by structures. This work provides an in-depth review of cutting-edge techniques employed for transient characterization of thermophysical properties at the micro/nanoscale scale. In terms of transient excitation, step Joule heating, step laser heating, pulsed laser heating, and frequency domain amplitude-modulated laser heating are covered. For thermal probing, electrical and Raman scattering-based physical principles are used. These techniques enable the measurement of thermal conductivity, thermal diffusivity, and specific heat from the sub-mm level down to the atomic level (single-atom thickness). This review emphasizes the advantages of these techniques over steady state techniques and their physics, challenges, and potential applications, highlighting their significance in unraveling the intricate thermal transport phenomena to the atomic level of 1D materials. 

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4. Ab initio nonadiabatic molecular dynamics of charge carriers in metal halide perovskites

   https://doi.org/10.1039/d1nr01990b  

   Li, Wei; She, Yalan; Vasenko, Andrey S.; Prezhdo, Oleg V. (June 2021, Nanoscale)

   Photoinduced nonequilibrium processes in nanoscale materials play key roles in photovoltaic and photocatalytic applications. This review summarizes recent theoretical investigations of excited state dynamics in metal halide perovskites (MHPs), carried out using a state-of-the-art methodology combining nonadiabatic molecular dynamics with real-time time-dependent density functional theory. The simulations allow one to study evolution of charge carriers at the ab initio level and in the time-domain, in direct connection with time-resolved spectroscopy experiments. Eliminating the need for the common approximations, such as harmonic phonons, a choice of the reaction coordinate, weak electron–phonon coupling, a particular kinetic mechanism, and perturbative calculation of rate constants, we model full-dimensional quantum dynamics of electrons coupled to semiclassical vibrations. We study realistic aspects of material composition and structure and their influence on various nonequilibrium processes, including nonradiative trapping and relaxation of charge carriers, hot carrier cooling and luminescence, Auger-type charge–charge scattering, multiple excitons generation and recombination, charge and energy transfer between donor and acceptor materials, and charge recombination inside individual materials and across donor/acceptor interfaces. These phenomena are illustrated with representative materials and interfaces. Focus is placed on response to external perturbations, formation of point defects and their passivation, mixed stoichiometries, dopants, grain boundaries, and interfaces of MHPs with charge transport layers, and quantum confinement. In addition to bulk materials, perovskite quantum dots and 2D perovskites with different layer and spacer cation structures, edge passivation, and dielectric screening are discussed. The atomistic insights into excited state dynamics under realistic conditions provide the fundamental understanding needed for design of advanced solar energy and optoelectronic devices. 

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5. The in-plane structure domain size of nm-thick MoSe ₂ uncovered by low-momentum phonon scattering

   https://doi.org/10.1039/d0nr09099a  

   Lin, Huan; Wang, Ridong; Zobeiri, Hamidreza; Wang, Tianyu; Xu, Shen; Wang, Xinwei (April 2021, Nanoscale)

   null (Ed.)

   Although 2D materials have been widely studied for more than a decade, very few studies have been reported on the in-plane structure domain (STD) size even though such a physical property is critical in determining the charge carrier and energy carrier transport. Grazing incidence X-ray diffraction (XRD) can be used for studying the in-plane structure of very thin samples, but it becomes more challenging to study few-layer 2D materials. In this work the nanosecond energy transport state-resolved Raman (nET-Raman) technique is applied to resolve this key problem by directly measuring the thermal reffusivity of 2D materials and determining the residual value at the 0 K-limit. Such a residual value is determined by low-momentum phonon scattering and can be directly used to characterize the in-plane STD size of 2D materials. Three suspended MoSe 2 (15, 50 and 62 nm thick) samples are measured using nET-Raman from room temperature down to 77 K. Based on low-momentum phonon scattering, the STD size is determined to be 58.7 nm and 84.5 nm for 50 nm and 62 nm thick samples, respectively. For comparison, the in-plane structure of bulk MoSe 2 that is used to prepare the measured nm-thick samples is characterized using XRD. It uncovers crystallite sizes of 64.8 nm in the (100) direction and 121 nm in the (010) direction. The STD size determined by our low momentum phonon scattering is close to the crystallite size determined by XRD, but still shows differences. The STD size by low-momentum phonon scattering is more affected by the crystallite sizes in all in-plane directions rather than that by XRD that is for a specific crystallographic orientation. Their close values demonstrate that during nanosheet preparation (peeling and transfer), the in-plane structure experiences very little damage. 

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