arXiv subjects

Shunda Chen

Publications and source records attributed to Shunda Chen.

At least 37 records · Page 2Linked to original sources

arXiv2021

Engineering thermal transport across layered graphene-MoS2 superlattices

Layering two-dimensional van der Waals materials provides unprecedented control over atomic placement, which could enable tailoring of vibrational spectra and heat flow at the sub-nanometer scale. Here, using spatially-resolved ultrafast thermoreflectance and spectroscopy, we uncover the design rules governing cross-plane heat transport in superlattices assembled from monolayers of graphene (G) and MoS2 (M). Using a combinatorial experimental approach, we probe nine different stacking sequences: G, GG, MG, GGG, GMG, GGMG, GMGG, GMMG, GMGMG and identify the effects of vibrational mismatch, interlayer adhesion, and junction asymmetry on thermal transport. Pure G sequences display signatures of quasi-ballistic transport, whereas adding even a single M layer strongly disrupts heat conduction. The experimental data are described well by molecular dynamics simulations which include thermal expansion, accounting for the effect of finite temperature on the interlayer spacing. The simulations show that a change of only 1.5% in the layer separation can lead to a nearly 100% increase of the thermal resistance. Using these design rules, we experimentally demonstrate a 5-layer GMGMG superlattice with an ultralow effective cross-plane thermal conductivity comparable to air, paving the way for a new class of thermal metamaterials with extreme properties.

cond-mat.mes-hall↗

arXiv2020

Short-range order in GeSn alloy

Group IV alloys have been long viewed as homogeneous random solid solutions since they were first perceived as Si-compatible, direct-band-gap semiconductors 30 years ago. Such a perception underlies the understanding, interpretation and prediction of alloys' properties. However, as the race to create scalable and tunable device materials enters a composition domain far beyond alloys' equilibrium solubility, a fundamental question emerges as to how random these alloys truly are. Here we show, by combining statistical sampling and large-scale ab initio calculations, that GeSn alloy, a promising group IV alloy for mid-infrared technology, exhibits a clear, short-range order for solute atoms within its entire composition range. Such short-range order is further found to substantially affect the electronic properties of GeSn. We demonstrate the proper inclusion of this short-range order through canonical sampling can lead to a significant improvement over previous predictions on alloy's band gaps, by showing an excellent agreement with experiments within the entire studied composition range. Our finding thus not only calls for an important revision of current structural model for group IV alloy, but also suggests short-range order may generically exist in different types of alloys.

cond-mat.mtrl-sci↗

arXiv2020

Mn-Intercalated MoSe$_2$ under pressure: electronic structure and vibrational characterization of a dilute magnetic semiconductor

Intercalation offers a promising way to alter the physical properties of two-dimensional (2D) layered materials. Here we investigate the electronic and vibrational properties of 2D layered MoSe$_2$ intercalated with atomic manganese at ambient and high pressure up to 7 GPa by Raman scattering and electronic structure calculations. The behavior of optical phonons is studied experimentally with a diamond anvil cell and computationally through density functional theory calculations. Experiment and theory show excellent agreement in optical phonon behavior. The previously Raman inactive A$_{2u}$ mode is activated and enhanced with intercalation and pressure, and a new Raman mode appears upon decompression, indicating a possible onset of a localized structural transition, involving the bonding or trapping of intercalant in 2D layered materials. Density functional theory calculations reveal a shift of Fermi level into the conduction band and spin polarization in Mn$_x$MoSe$_2$ that increases at low Mn concentration and low pressure. Our results suggest that intercalation and pressurization of van der Waals materials may allow one to obtain dilute magnetic semiconductors with controllable properties, providing a viable route for the development of new materials for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2020

Transferability of neural network potentials for varying stoichiometry: phonons and thermal conductivity of Mn$_x$Ge$_y$ compounds

Germanium manganese compounds exhibit a variety of stable and metastable phases with different stoichiometry. These materials entail interesting electronic, magnetic and thermal properties both in their bulk form and as heterostructures. Here we develop and validate a transferable machine learning potential, based on the high-dimensional neural network formalism, to enable the study of Mn$_x$Ge$_y$ materials over a wide range of compositions. We show that a neural network potential fitted on a minimal training set reproduces successfully the structural and vibrational properties and the thermal conductivity of systems with different local chemical environments, and it can be used to predict phononic effects in nanoscale heterostructures.

cond-mat.mtrl-sci↗

arXiv2019

Influence of Boundaries and Thermostatting on Nonequilibrium Molecular Dynamics Simulations of Heat Conduction in Solids

Nonequilibrium molecular dynamics (NEMD) has been extensively used to study thermal transport at various length scales in many materials. In this method, two local thermostats at different temperatures are used to generate a nonequilibrium steady state with a constant heat flux. Conventionally, the thermal conductivity of a finite system is calculated as the ratio between the heat flux and the temperature gradient extracted from the linear part of the temperature profile away from the local thermostats. Here we show that, with a proper choice of the thermostat, the nonlinear part of the temperature profile should actually not be excluded in thermal transport calculations. We compare NEMD results against those from the atomistic Green's function method in the ballistic regime, and those from the homogeneous nonequilibrium molecular dynamics method in the ballistic-to-diffusive regime. These comparisons suggest that in all the transport regimes, one should directly calculate the thermal conductance from the temperature difference between the heat source and sink and, if needed, convert it to the thermal conductivity by multiplying it with the system length. Furthermore, we find that the Langevin thermostat outperforms the Nosé-Hoover (chain) thermostat in NEMD simulations because of its stochastic and local nature. We show that this is particularly important for studying asymmetric carbon-based nanostructures, for which the Nosé-Hoover thermostat can produce artifacts leading to unphysical thermal rectification. Our findings are important to obtain correct results from molecular dynamics simulations of nanoscale heat transport as the accuracy of the interatomic potentials is rapidly improving.

cond-mat.mes-hall↗

arXiv2019

Strongly Tunable Anisotropic Thermal Transport in MoS2 by Strain and Lithium Intercalation: First--Principles Calculations

The possibility of tuning the vibrational properties and the thermal conductivity of layered van der Waals materials either chemically or mechanically paves the way to significant advances in nanoscale heat management. Using first-principles calculations we investigate the modulation of heat transport in MoS2 by lithium intercalation and cross-plane strain. We find that both the in-plane and cross-plane thermal conductivity (kr, kz) of MoS2 are extremely sensitive to both strain and electrochemical intercalation. Combining lithium intercalation and strain, the in-plane and cross-plane thermal conductivity can be tuned over one and two orders of magnitude, respectively. Furthermore, since kr and kz respond in different ways to intercalation and strain, the thermal conductivity anisotropy can be modulated by two orders of magnitude. The underlying mechanisms for such large tunability of the anisotropic thermal conductivity of \Mos are explored by computing and analyzing the dispersion relations, group velocities, relaxation times and mean free paths of phonons. Since both intercalation and strain can be applied reversibly, their stark effect on thermal conductivity can be exploited to design novel phononic devices, as well as for thermal management in MoS2-based electronic and optoelectronic systems.

cond-mat.mtrl-sci↗

arXiv2019

Quasi-ballistic thermal transport across MoS$_2$ thin films

Layered two-dimensional (2D) materials have highly anisotropic thermal properties between the in-plane and cross-plane directions. In general, it is thought that cross-plane thermal conductivities ($κ_z$) are low, and therefore c-axis phonon mean free paths (MFPs) are small. Here, we measure $κ_z$ across MoS$_2$ films of varying thickness (20 to 240 nm) and uncover evidence of very long c-axis phonon MFPs at room temperature in these layered semiconductors. Experimental data obtained using time-domain thermoreflectance (TDTR) are in good agreement with first-principles density functional theory (DFT). These calculations reveal that ~50% of the heat is carried by phonons with MFP >200 nm, exceeding kinetic theory estimates by nearly two orders of magnitude. Because of quasi-ballistic effects, the $κ_z$ of nanometer thin films of MoS$_2$ scales with their thickness and the volumetric thermal resistance asymptotes to a non-zero value, ~10 m$^{2}$KGW$^{-1}$. This contributes as much as 30% to the total thermal resistance of a 20 nm thick film, the rest being limited by thermal interface resistance with the SiO$_2$ substrate and top-side aluminum transducer. These findings are essential for understanding heat flow across nanometer-thin films of MoS$_2$ for optoelectronic and thermoelectric applications.

cond-mat.mes-hall↗

arXiv2019

An electrochemical thermal transistor

The ability to actively regulate heat flow at the nanoscale could be a game changer for applications in thermal management and energy harvesting. Such a breakthrough could also enable the control of heat flow using thermal circuits, in a manner analogous to electronic circuits. Here we demonstrate switchable thermal transistors with an order of magnitude thermal on/off ratio, based on reversible electrochemical lithium intercalation in MoS2 thin films. We use spatially-resolved time-domain thermoreflectance to map the lithium ion distribution during device operation, and atomic force microscopy to show that the lithiated state correlates with increased thickness and surface roughness. First principles calculations reveal that the thermal conductance modulation is due to phonon scattering by lithium rattler modes, c-axis strain, and stacking disorder. This study lays the foundation for electrochemically-driven nanoscale thermal regulators, and establishes thermal metrology as a useful probe of spatio-temporal intercalant dynamics in nanomaterials.

physics.app-ph↗

arXiv2017

An efficient thermal diode with ballistic spacer

Thermal rectification is of importance not only for fundamental physics, but also for potential applications in thermal manipulations and thermal management. However, thermal rectification effect usually decays rapidly with system size. Here, we show that a mass-graded system, with two diffusive leads separated by a ballistic spacer, can exhibit large thermal rectification effect, with the rectification factor independent of system size. The underlying mechanism is explained in terms of the effective size-independent thermal gradient and the match/mismatch of the phonon bands. We also show the robustness of the thermal diode upon variation of the model's parameters. Our finding suggests a promising way for designing realistic efficient thermal diodes.

cond-mat.stat-mech↗

arXiv2015

Connection between heat diffusion and heat conduction in one-dimensional systems

Heat and energy are conceptually different, but often are assumed to be the same without justification. An effective method for investigating diffusion properties in equilibrium systems is discussed. With this method, we demonstrate that for one-dimensional systems, using the indices of particles as the space variable , which has been accepted as a convention, may lead to misleading conclusions. We then show that though in one-dimensional systems there is no general connection between energy diffusion and heat conduction, however, a general connection between heat diffusion and heat conduction may exist. Relaxation behavior of local energy current fluctuations and that of local heat current fluctuations are also studied. We find that they are significantly different, though the global energy current equals the globe heat current.

cond-mat.stat-mech↗

arXiv2015

Key role of asymmetric interactions in low-dimensional heat transport

We study the heat current autocorrelation function (HCAF) in one-dimensional, momentum-conserving lattices. In particular, we explore if there is any relation between the decaying characteristics of the HCAF and asymmetric interparticle interactions. The Lennard-Jones model is intensively investigated in view of its significance to applications. It is found that in wide ranges of parameters, the HCAF decays faster than power-law manners, and in some cases it decays even exponentially. Following the Green-Kubo formula, the fast decay of HCAF implies the convergence of heat conductivity, which is also corroborated by numerical simulations. In addition, with a comparison to the Fermi-Pasta-Ulam-$β$ model of symmetric interaction, the HCAF of the Fermi-Pasta-Ulam-$α$-$β$ model of asymmetric interaction is also investigated. Our study suggests that, in certain ranges of parameters, the decaying behavior of the HCAF is correlated to the asymmetry degree of interaction.

cond-mat.stat-mech↗

arXiv2015

Thermoelectricity of interacting particles: A numerical approach

A method for computing the thermopower in interacting systems is proposed. This approach, which relies on Monte Carlo simulations, is illustrated first for a diatomic chain of hard-point elastically colliding particles and then in the case of a one-dimensional gas with (screened) Coulomb interparticle interaction. Numerical simulations up to $N>10^4$ particles confirm the general theoretical arguments for momentum-conserving systems and show that the thermoelectric figure of merit increases linearly with the system size.

cond-mat.stat-mech↗

arXiv2015

Ingredients for an efficient thermal diode

We provide convincing empirical evidence that long range interactions strongly enhance the rectification effect which takes place in mass graded systems. Even more importantly the rectification does not decrease with the increase of the system size. Large rectification is obtained also for the equal mass case and with graded on-site potential. These results allow to overcome current limitations of the rectification mechanism and open the way for a realistic implementation of efficient thermal diodes.

cond-mat.stat-mech↗

arXiv2014

Non-integrability and the Fourier heat conduction law

We study in momentum-conserving systems, how nonintegrable dynamics may affect thermal transport properties. As illustrating examples, two one-dimensional (1D) diatomic chains, representing 1D fluids and lattices, respectively, are numerically investigated. In both models, the two species of atoms are assigned two different masses and are arranged alternatively. The systems are nonintegrable unless the mass ratio is one. We find that when the mass ratio is slightly different from one, the heat conductivity may keep significantly unchanged over a certain range of the system size and as the mass ratio tends to one, this range may expand rapidly. These results establish a new connection between the macroscopic thermal transport properties and the underlying dynamics.

cond-mat.stat-mech↗

arXiv2014

Finite-size effects on current correlation functions

We study why the calculation of current correlation functions (CCFs) still suffers from finite size effects even when the periodic boundary condition is taken. Two important one dimensional, momentum conserving systems are investigated as examples. Intriguingly, it is found that the state of a system recurs in the sense of microcanonical ensemble average, and such recurrence may result in oscillations in CCFs. Meanwhile, we find that the sound mode collisions induce an extra time decay in a current so that its correlation function decays faster (slower) in a smaller (larger) system. Based on these two unveiled mechanisms, a procedure for correctly evaluating the decay rate of a CCF is proposed, with which our analysis suggests that the global energy CCF decays as $\sim t^{-\frac{2}{3}}$ in the diatomic hard-core gas model and in a manner close to $\sim t^{-\frac{1}{2}}$ in the Fermi-Pasta-Ulam-$β$ model.

cond-mat.stat-mech↗

arXiv2013

Why asymmetric interparticle interaction can result in convergent heat conductivity

We show that the asymmetric inter-particle interactions may induce rapid decay of heat current autocorrelation in one-dimensional momentum conserving lattices. When the asymmetry degree and the temperature are appropriate, the decay is sufficient rapid for resulting a convergence conductivity practically. To understand the underlying mechanism, we further studied the relaxation behavior of the hydrodynamic modes. It is shown that for lattice with symmetric potential, the heat mode relaxs in the superdiffusive manner, while in the case of asymmetric potential, the heat mode may relax in the normal manner.

cond-mat.stat-mech↗

arXiv2013

Diffusion of heat, energy, momentum, and mass in one-dimensional systems

We study diffusion processes of local fluctuations of heat, energy, momentum, and mass in three paradigmatic one-dimensional systems. For each system, diffusion processes of four physical quantities are simulated and the cross correlations between them are investigated. We find that, in all three systems, diffusion processes of energy and mass can be perfectly expressed as a linear combination of those of heat and momentum, suggesting that diffusion processes of heat and momentum may represent the heat mode and the sound mode in the hydrodynamic theory. In addition, the dynamic structure factor, which describes the diffusion behavior of local mass density fluctuations, is in general insufficient for probing diffusion processes of other quantities because in some cases there is no correlation between them. We also find that the diffusion behavior of heat can be qualitatively different from that of energy, and, as a result, previous studies trying to relate heat conduction to energy diffusion should be revisited.

cond-mat.stat-mech↗

arXiv2013

Breakdown of effective phonon theory in one-dimensional chains with asymmetric interactions

Phonons are universal language for solid state theory. Effective phonon theory (self-consistent harmonic approximation) have been extensively used to access the weakly nonlinear effect in solid materials, which are standard content in textbook. In this manuscript, we test the effective phonon theory in one-dimensional chains with asymmetric interactions. It is found that simulation results agree well with theoretical predictions for symmetric cases, while significantly deviate from theoretical predictions for asymmetric cases. Our results imply the asymmetric interaction can provide stronger phonon-phonon interaction, which lead to break down of the effective phonon theory.

cond-mat.stat-mech↗