arXiv subjects

Yee Kan Koh

Publications and source records attributed to Yee Kan Koh.

15 recordsLinked to original sources

arXiv2025

Direct Joule-Heated Non-Equilibrium Synthesis Enables High Performing Thermoelectrics

High-throughput synthesis of bulk inorganic materials is crucial for accelerating functional materials discovery but is hindered by slow, energy-intensive solid-state methods. We introduce Direct Joule-Heated Synthesis (DJS), a rapid, single-step and scalable solid-state synthesis technique achieving a $10^5$-fold speedup and 20,000x energy efficiency improvement over conventional synthesis. DJS enables the synthesis of dense, bulk chalcogenides ($\mathrm{Bi_{0.5}Sb_{1.5}Te_3}$, $\mathrm{AgSbTe_2}$), achieving a zT of 2.3 at 573 K in optimally Cd/Se co-doped $\mathrm{AgSbTe_2}$, one of the highest for polycrystalline materials at this temperature. DJS enables optimal co-doping and rapid, non-equilibrium solidification, producing lamellar microstructures, interfacial regions, and cation-ordered nanodomains that scatter all-scale phonons, achieving ultralow lattice thermal conductivity (~0.2 $W m^{-1} K^{-1}$ at 573 K). DJS establishes a new benchmark for scalable and fast synthesis, accelerating functional material discovery.

cond-mat.mtrl-sci↗

arXiv2022

Non-equilibrium Phonon Thermal Resistance at MoS2/Oxide and Graphene/Oxide Interfaces

Accurate measurements and physical understanding of thermal boundary resistance (R) of two-dimensional (2D) materials are imperative for effective thermal management of 2D electronics and photonics. In previous studies, heat dissipation from 2D material devices was presumed to be dominated by phonon transport across the interfaces. In this study, we find that in addition to phonon transport, thermal resistance between non-equilibrium phonons in the 2D materials could play a critical role too when the 2D material devices are internally self-heated, either optically or electrically. We accurately measure R of oxide/MoS2/oxide and oxide/graphene/oxide interfaces for three oxides (SiO2, HfO2, Al2O3) by differential time-domain thermoreflectance (TDTR). Our measurements of R across these interfaces with external heating are 2-to-4 times lower than previously reported R of the similar interfaces measured by Raman thermometry with internal self-heating. Using a simple model, we show that the observed discrepancy can be explained by an additional internal thermal resistance (Rint) between non-equilibrium phonons present during Raman measurements. We subsequently estimate that for MoS2 and graphene, Rint is about 31 and 22 m2 K/GW, respectively. The values are comparable to the thermal resistance due to finite phonon transmission across interfaces of 2D materials and thus cannot be ignored in the design of 2D material devices. Moreover, the non-equilibrium phonons also lead to a different temperature dependence than that by phonon transport. As such, our work provides important insights into physical understanding of heat dissipation in 2D material devices.

physics.app-ph↗

arXiv2018

Anisotropic model with truncated linear dispersion for lattice and interfacial thermal transport in layered materials

Recently, an anisotropic Debye model [Dames et al., Physical Review B 87, 12 (2013)] was proposed for calculations of the interfacial thermal conductance and the minimum thermal conductivity of graphite-like layered materials. Despite successes of the model in explaining heat transport mechanisms in layered materials (e.g., phonon focusing in highly anisotropic materials), the anisotropic Debye model assumes a phonon dispersion with unrealistic speeds of sounds especially for the flexural (ZA) phonons and overestimated cutoffs for all phonon branches. The deficiencies lead to substantially underestimated phonon irradiation for low-frequency phonons. Here, we develop an anisotropic model with truncated linear dispersion that resembles the real phonon dispersion, using speeds of sounds derived from elastic constants and cutoff frequencies derived from Brillouin zone boundaries. We also employ a piecewise linear function for the ZA phonons. Our model correctly calculates the phonon irradiation over a wide temperature range, verifying the accuracy of our model.We compare calculations of our and the Dames models to measurements of thermal conductivity of graphite and thermal conductance of metal/graphite interfaces, and find that the two models differ significantly for heat transport across the basal planes in graphite even at high temperatures. Our work thus provides a convenient analytical tool to study the phonon transport properties in layered materials.

physics.app-ph↗

arXiv2018

Tuning electronic heat transport in graphene/metal heterostructures with ultralow thermal conductivity

Prior ultralow thermal conductivity materials are not suitable for thermoelectric applications due to the limited electronic transport in the materials. Here, we present a new class of ultralow thermal conductivity materials with substantial electronic heat transport. Our samples are graphene/metal heterostructures of transferred graphene and ultrathin metal films (Pd, Au and Ni) deposited by either thermal evaporation or rf magnetron sputtering. For the evaporated samples, we achieve an ultralow thermal conductivity of 0.06 W m-1 K-1, with phonons as the dominant heat carriers. The ultralow thermal conductivity is due to a huge disparity in phonon energy in graphene and metals. Interestingly, for the sputtered samples, we find that about 50 % of heat is carried by electrons, even when thermal conductivity is about 0.1 W m-1 K-1. We attribute the electronic contribution to transmission of electrons across atomic-scale pinholes in graphene. With the ultralow thermal conductivity and substantial electronic transport, the new materials could be explored for thermoelectric applications.

cond-mat.mtrl-sci↗

arXiv2018

Achieving huge thermal conductance of metallic nitride on graphene through enhanced elastic and inelastic phonon transmission

Low thermal conductance of metal contacts is one of the main challenges in thermal management of nanoscale devices of graphene and other 2D materials. Previous attempts to search for metal contacts with high thermal conductance yielded limited success due to incomplete understanding of the origins of the low thermal conductance. In this paper, we carefully study the intrinsic thermal conductance across metal/graphene/metal interfaces to identify the heat transport mechanisms across graphene interfaces. We find that unlike metal contacts on diamond, the intrinsic thermal conductance of most graphene interfaces (except Ti and TiNx) is only about 50 % of the phonon radiation limit, suggesting that heat is carried across graphene interfaces mainly through elastic transmission of phonons. We thus propose a convenient approach to substantially enhance the phononic heat transport across metal contacts on graphene, by better matching the energy of phonons in metals and graphene, e.g., using metallic nitrides. We test the idea with TiNx, with phonon frequencies of up to 1.18*10^14 rad/s, 47 % of the highest phonon frequencies in graphene of 2.51*10^14 rad/s . Interestingly, we obtain a huge thermal conductance of 270 MW m-2 K-1 for TiNx/graphene interfaces, which is about 140 % of the phonon radiation limit. The huge thermal conductance could be partially attributed to inelastic phonon transport across the TiNx/graphene interface. Our work provides guidance for the search for good metal contacts on 2D materials and devices.

physics.app-ph↗

arXiv2018

Dislocation-induced thermal transport anisotropy in single-crystal group-III nitride films

Dislocations, one-dimensional lattice imperfections, are common to technologically important materials such as III-V semiconductors, and adversely affect heat dissipation in e.g., nitride-based high-power electronic devices. For decades, conventional models based on nonlinear elasticity theory have predicted this thermal resistance is only appreciable when heat flux is perpendicular to the dislocations. However, this dislocation-induced anisotropic thermal transport has yet to be seen experimentally. In this study, we measure strong thermal transport anisotropy governed by highly oriented threading dislocation arrays along the cross-plane direction in micron-thick, single-crystal indium nitride (InN) films. We find that the cross-plane thermal conductivity is more than tenfold higher than the in-plane thermal conductivity at 80 K when the dislocation density is on the order of ~3x10^10 cm^-2. This large anisotropy is not predicted by the conventional models. With enhanced understanding of dislocation-phonon interactions, our results open new regimes for tailoring anisotropic thermal transport with line defects, and will facilitate novel methods for directed heat dissipation in thermal management of diverse device applications.

cond-mat.mtrl-sci↗

arXiv2018

Interfacial Phonon Scattering and Transmission Loss in >1 um Thick Silicon-on-insulator Thin Films

Scattering of phonons at boundaries of a crystal (grains, surfaces, or solid/solid interfaces) is characterized by the phonon wavelength, the angle of incidence, and the interface roughness, as historically evaluated using a specularity parameter p formulated by Ziman [J. M. Ziman, Electrons and Phonons (Clarendon Press, Oxford, 1960)]. This parameter was initially defined to determine the probability of a phonon specularly reflecting or diffusely scattering from the rough surface of a material. The validity of Ziman's theory as extended to solid/solid interfaces has not been previously validated. To better understand the interfacial scattering of phonons and to test the validity of Ziman's theory, we precisely measured the in-plane thermal conductivity of a series of Si films in silicon-on-insulator (SOI) wafers by time-domain thermoreflectance (TDTR) for a Si film thickness range of 1 - 10 μm and a temperature range of 100 - 300 K. The Si/SiO2 interface roughness was determined to be 0.11+/-0.04 nm using transmission electron microscopy (TEM). Furthermore, we compared our in-plane thermal conductivity measurements to theoretical calculations that combine first-principles phonon transport with Ziman's theory. Calculations using Ziman's specularity parameter significantly overestimate values from the TDTR measurements. We attribute this discrepancy to phonon transmission through the solid/solid interface into the substrate, which is not accounted for by Ziman's theory for surfaces. We derive a simple expression for the specularity parameter at solid/amorphous interfaces and achieve good agreement between calculations and measurement values.

cond-mat.mes-hall↗

arXiv2017

Negligible electronic contribution to heat transfer across intrinsic metal/graphene interfaces

Despite the importance of high thermal conductance (i.e. low thermal resistance) of metal contacts to thermal management of graphene devices, prior reported thermal conductance of metal/graphene interfaces are all relatively low, only 20-40 MW m$^{-2}$ K$^{-1}$. One possible route to improve the thermal conductance ($G$) of metal/graphene interfaces is through additional heat conduction by electrons, since graphene can be easily doped by metals. In this paper, we evaluate the electronic heat conduction across metal/graphene interfaces by measuring the thermal conductance of Pd/transferred graphene (trG)/Pd interfaces, prepared by either thermal evaporation or radio-frequency (rf) magnetron sputtering, over a wide temperature range of 80 to 500 K. We find that for the samples prepared by thermal evaporation, the thermal conductance of Pd/trG/Pd is 42 MW m$^{-2}$ K$^{-1}$. The thermal conductance only weakly depends on temperature, which suggests that heat is predominantly carried by phonons across the intrinsic Pd/graphene interface. However, for Pd/trG/Pd samples with the top Pd films deposited by rf magnetron sputtering, we observe a significant increment of thermal conductance from the intrinsic value of 42 MW m$^{-2}$ K$^{-1}$ to 300 MW m$^{-2}$ K$^{-1}$, and $G$ is roughly proportional to $T$. We attribute the enhancement of thermal conductance to an additional channel of heat transport by electrons via atomic-scale pinholes formed in the graphene during the sputtering process. We thus conclude that electrons play a negligible role in heat conduction across intrinsic interfaces of metal and pristine graphene, and the contribution of electrons is only substantial if graphene is damaged.

cond-mat.mes-hall↗

arXiv2016

Temperature dependence of anisotropic thermal conductivity tensor of bulk black phosphorus

To date, the intrinsic thermal conductivity tensor of bulk black phosphorus (BP), an important 2D material, is still unknown, since recent studies focus on BP flakes not on bulk BP. Here we report the anisotropic thermal conductivity tensor of bulk BP, for temperature range 80 - 300 K. Our measurements are similar to prior measurements on submicron BP flakes along zigzag and armchair axes, but are >25% higher in the through-plane axis, suggesting that phonon mean-free-paths are substantially longer in the through-plane direction. We find that despite the anisotropy in thermal conductivity, phonons are predominantly scattered by the same Umklapp processes in all directions. We also find that the phonon relaxation time is rather isotropic in the basal planes, but is highly anisotropic in the through-plane direction. Our work advances fundamental knowledge of anisotropic scattering of phonons in BP and is an important benchmark for future studies on thermal properties of BP nanostructures.

cond-mat.mtrl-sci↗

arXiv2016

Role of remote interfacial phonon (RIP) scattering in heat transport across graphene/SiO2 interfaces

Heat transfer across interfaces of graphene and polar dielectrics (e.g. SiO2) could be mediated by direct phonon coupling, as well as electronic coupling with remote interfacial phonons (RIPs). To understand the relative contribution of each component, we develop a new pump-probe technique, called voltage-modulated thermoreflectance (VMTR), to accurately measure the change of interfacial thermal conductance under an electrostatic field. We employed VMTR on top gates of graphene field-effect transistors and find that the thermal conductance of SiO2/graphene/SiO2 interfaces increases by up to ΔG=0.8 MW m-2 K-1 under electrostatic fields of <0.2 V nm-1 . We propose two possible explanations for the observed ΔG. First, since the applied electrostatic field induces charge carriers in graphene, our VMTR measurements could originate from heat transfer between the charge carriers in graphene and RIPs in SiO2. Second, the increase in heat conduction could be caused by better conformity of graphene interfaces un-der electrostatic pressure exerted by the induced charge carriers. Regardless of the origins of the observed ΔG, our VMTR measurements establish an upper limit for heat transfer from unbiased graphene to SiO2 substrates via RIP scattering; i.e., only <2 % of the interfacial heat transport is facilitated by RIP scattering even at a carrier concentration of 4x10^12 cm-2.

cond-mat.mes-hall↗

arXiv2016

Accurate Measurements of Cross-plane Thermal Conductivity of Thin Films by Dual-Frequency Time-Domain Thermoreflectance (TDTR)

Accurate measurements of the cross-plane thermal conductivity Λ_cross of a high-thermal-conductivity thin film on a low-thermal-conductivity (Λ_s) substrate (e.g., Λ_cross/Λ_s>20) are challenging, due to the low thermal resistance of the thin film compared to that of the substrate. In principle, Λ_cross could be measured by time-domain thermoreflectance (TDTR), using a high modulation frequency f_h and a large laser spot size. However, with one TDTR measurement at f_h, the uncertainty of the TDTR measurement is usually high due to low sensitivity of TDTR signals to Λ_cross and high sensitivity to the thickness h_Al of Al transducer deposited on the sample for TDTR measurements. We observe that in most TDTR measurements, the sensitivity to h_Al only depends weakly on the modulation frequency f. Thus, we performed an additional TDTR measurement at a low modulation frequency f_0, such that the sensitivity to h_Al is comparable but the sensitivity to Λcross is near zero. We then analyze the ratio of the TDTR signals at f_h to that at f_0, and thus significantly improve the accuracy of our Λcross measurements. As a demonstration of the dual-frequency approach, we measured the cross-plane thermal conductivity of a 400-nm-thick nickel-iron alloy film and a 3-μm-thick Cu film, both with an accuracy of ~10%. The dual-frequency TDTR approach is useful for future studies of thin films.

cond-mat.mtrl-sci↗

arXiv2015

Improved topological conformity enhances heat conduction across metal contacts on transferred graphene

Thermal conductance of metal contacts on transferred graphene (trG) could be significantly reduced from the intrinsic value of similar contacts on as-grown graphene (grG), due to additional resistance by increased roughness, residues, oxides and voids. In this paper, we compare the thermal conductance (G) of Al/trG/Cu interfaces with that of Al/grG/Cu interfaces to understand heat transfer across metal contacts on transferred graphene. Our samples are polycrystalline graphene grown on Cu foils by chemical vapor deposition (CVD) and CVD-grown graphene transferred to evaporated Cu thin films. We find that for the Al/grG/Cu interfaces of as-grown CVD graphene, G=31 MW m^{-2} K^{-1} at room temperature, two orders of magnitude lower than that of Al/Cu interfaces. For most as-transferred graphene on Cu films, G=20 MW m^{-2} K^{-1}, 35% lower than that of as-grown CVD graphene. We carefully rule out the contributions of residues, native oxides and interfaces roughness, and attribute the difference in the thermal conductance of as-grown and as-transferred CVD graphene to different degrees of conformity of graphene to the Cu substrates. We find that a contact area of 50% only reduces the thermal conductance by 35%, suggesting that a small amount of heat transfer occurs across voids at graphene interfaces. We successfully improve the conformity of the as-transferred graphene to the substrates by annealing the samples at 300°C, and thus enhance the thermal conductance of the transferred graphene to the intrinsic value. From the temperature dependence measurements of G of Al/trG/Cu and Al/grG/Cu interfaces, we also confirm that phonons are the dominant heat carries across the metal/graphene/metal interfaces despite a substantial carrier concentration of 3x10^{12} cm^{-2} induced in the graphene.

cond-mat.mtrl-sci↗

arXiv2015

The role of low-energy phonons with mean-free-paths >0.8 um in heat conduction in silicon

Despite recent progress in the first-principles calculations and measurements of phonon mean-free-paths (MFPs), contribution of low-energy phonons to heat conduction in silicon is still inconclusive, as exemplified by the discrepancies between different first-principles calculations. Here we investigate the contribution of low-energy phonons with MFP>0.8 um by accurately measuring the cross-plane thermal conductivity of crystalline silicon films by time-domain thermoreflectance (TDTR), over a wide range of film thickness 1-10 um and temperature 100-300 K. We employ a dual-frequency TDTR approach to improve the accuracy of our cross-plane thermal conductivity measurements. We find from our cross-plane thermal conductivity measurements that phonons with MFP>0.8 um contribute 53 W/m-K (37%) to heat conduction in Si at 300 K while phonons with MFP>3 um contribute 523 W/m-K (61%) at 100 K, >20% lower than the first-principles predictions by Lindsay et al. of 68 W/m-K (47%) and 695 W/m-K (77%), respectively. Using a relaxation times approximation (RTA) model, we demonstrate that macroscopic damping (e.g., Akhieser's damping) eliminates the contribution of phonons with mean-free-paths >30 um at 300 K, which contributes 15 W/m-K (10%) to heat conduction in Si according to Lindsay et al. Thus we propose that omission of the macroscopic damping for low-energy phonons in the first-principles calculations could be one of the possible explanations for the observed discrepancy between our measurements and calculations by Lindsay et al. Our work provides an important benchmark for future measurements and calculations of the distribution of phonon mean-free-paths in crystalline silicon.

cond-mat.mtrl-sci↗

arXiv2010

Heat Conduction across Monolayer and Few-Layer Graphenes

We report the thermal conductance G of Au/Ti/graphene/SiO2 interfaces (graphene layers 1 < n < 10) typical of graphene transistor contacts. We find G ~ 25 MW m-2 K-1 at room temperature, four times smaller than the thermal conductance of a Au/Ti/SiO2 interface, even when n = 1. We attribute this reduction to the thermal resistance of Au/Ti/graphene and graphene/SiO2 interfaces acting in series. The temperature dependence of G from 50 < T < 500 K also indicates that heat is predominantly carried by phonons through these interfaces. Our findings indicate that metal contacts can limit not only electrical transport, but also thermal dissipation from sub-micron graphene devices.

cond-mat.mes-hall↗

arXiv2010

Reliably Counting Atomic Planes of Few-Layer Graphene (n>4)

We demonstrate a reliable technique for counting atomic planes (n) of few-layer graphene (FLG) on SiO2/Si substrates by Raman spectroscopy. Our approach is based on measuring the ratio of the integrated intensity of the G graphene peak and the optical phonon peak of Si, I(G)/I(Si), and is particularly useful in the range n>4 where few methods exist. We compare our results with atomic force microscopy (AFM) measurements and Fresnel equation calculations. Lastly, we apply our method to unambiguously identify n of FLG devices and find that the mobility (~2000 cm2 V-1 s-1) is independent of layer thickness for n>4.

cond-mat.mes-hall↗