A new elliptical-beam method based on time-domain thermoreflectance (TDTR) to measure the in-plane anisotropic thermal conductivity and its comparison with the beam-offset method.

Materials lacking in-plane symmetry are ubiquitous in a wide range of applications such as electronics, thermoelectrics, and high-temperature superconductors, in all of which the thermal properties of the materials play a critical part. However, very few experimental techniques can be used to measure in-plane anisotropic thermal conductivity. A beam-offset method based on time-domain thermoreflectance (TDTR) was previously proposed to measure in-plane anisotropic thermal conductivity. However, a detailed analysis of the beam-offset method is still lacking. Our analysis shows that uncertainties can be large if the laser spot size or the modulation frequency is not properly chosen. Here we propose an alternative approach based on TDTR to measure in-plane anisotropic thermal conductivity using a highly elliptical pump (heating) beam. The highly elliptical pump beam induces a quasi-one-dimensional temperature profile on the sample surface that has a fast decay along the short axis of the pump beam. The detected TDTR signal is exclusively sensitive to the in-plane thermal conductivity along the short axis of the elliptical beam. By conducting TDTR measurements as a function of delay time with the rotation of the elliptical pump beam to different orientations, the in-plane thermal conductivity tensor of the sample can be determined. In this work, we first conduct detailed signal sensitivity analyses for both techniques and provide guidelines in determining the optimal experimental conditions. We then compare the two techniques under their optimal experimental conditions by measuring the in-plane thermal conductivity tensor of a ZnO [11-20] sample. The accuracy and limitations of both methods are discussed.

High temperature thermal management with boron nitride nanosheets.

The rapid development of high power density devices requires more efficient heat dissipation. Recently, two-dimensional layered materials have attracted significant interest due to their superior thermal conductivity, ease of production and chemical stability. Among them, hexagonal boron nitride (h-BN) is electrically insulating, making it a promising thermal management material for next-generation electronics. In this work, we demonstrated that an h-BN thin film composed of layer-by-layer laminated h-BN nanosheets can effectively enhance the lateral heat dissipation on the substrate. We found that by using the BN-coated glass instead of bare glass as the substrate, the highest operating temperature of a reduced graphene oxide (RGO) based device could increase from 700 °C to 1000 °C, and at the same input power, the operating temperature of the RGO device is effectively decreased. The remarkable performance improvement using the BN coating originates from its anisotropic thermal conductivity: a high in-plane thermal conductivity of 14 W m-1 K-1 for spreading and a low cross-plane thermal conductivity of 0.4 W m-1 K-1 to avoid a hot spot right underneath the device. Our results provide an effective approach to improve the heat dissipation in integrated circuits and high power devices.

Time-domain thermoreflectance (TDTR) measurements of anisotropic thermal conductivity using a variable spot size approach.

It is challenging to characterize thermal conductivity of materials with strong anisotropy. In this work, we extend the time-domain thermoreflectance (TDTR) method with a variable spot size approach to simultaneously measure the in-plane (Kr) and the through-plane (Kz) thermal conductivity of materials with strong anisotropy. We first determine Kz from the measurement using a larger spot size, when the heat flow is mainly one-dimensional along the through-plane direction, and the measured signals are only sensitive to Kz. We then extract the in-plane thermal conductivity Kr from a second measurement using the same modulation frequency but with a smaller spot size, when the heat flow becomes three-dimensional, and the signal is sensitive to both Kr and Kz. By choosing the same modulation frequency for the two sets of measurements, we can avoid potential artifacts introduced by the frequency-dependent Kz, which we have found to be non-negligible, especially for some two-dimensional layered materials like MoS2. After careful evaluation of the sensitivity of a series of hypothetical samples, we provided guidelines on choosing the most appropriate laser spot size and modulation frequency that yield the smallest uncertainty, and established a criterion for the range of thermal conductivity that can be measured reliably using our proposed variable spot size TDTR approach. We have demonstrated this variable spot size TDTR approach on samples with a wide range of in-plane thermal conductivity, including fused silica, rutile titania (TiO2 [001]), zinc oxide (ZnO [0001]), molybdenum disulfide (MoS2), hexagonal boron nitride (h-BN), and highly ordered pyrolytic graphite.

Probing Anisotropic Thermal Conductivity of Transition Metal Dichalcogenides MX2 (M = Mo, W and X = S, Se) using Time-Domain Thermoreflectance.

Transition metal dichalcogenides (TMDs) are a group of layered 2D semiconductors that have shown many intriguing electrical and optical properties. However, the thermal transport properties in TMDs are not well understood due to the challenges in characterizing anisotropic thermal conductivity. Here, a variable-spot-size time-domain thermoreflectance approach is developed to simultaneously measure both the in-plane and the through-plane thermal conductivity of four kinds of layered TMDs (MoS2 , WS2 , MoSe2 , and WSe2 ) over a wide temperature range, 80-300 K. Interestingly, it is found that both the through-plane thermal conductivity and the Al/TMD interface conductance depend on the modulation frequency of the pump beam for all these four compounds. The frequency-dependent thermal properties are attributed to the nonequilibrium thermal resistance between the different groups of phonons in the substrate. A two-channel thermal model is used to analyze the nonequilibrium phonon transport and to derive the intrinsic thermal conductivity at the thermal equilibrium limit. The measurements of the thermal conductivities of bulk TMDs serve as an important benchmark for understanding the thermal conductivity of single- and few-layer TMDs.

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 Λcross of a high-thermal-conductivity thin film on a low-thermal-conductivity (Λs) substrate (e.g., Λcross/Λs > 20) are challenging, due to the low thermal resistance of the thin film compared with that of the substrate. In principle, Λcross could be measured by time-domain thermoreflectance (TDTR), using a high modulation frequency fh and a large laser spot size. However, with one TDTR measurement at fh, the uncertainty of the TDTR measurement is usually high due to low sensitivity of TDTR signals to Λcross and high sensitivity to the thickness hAl of Al transducer deposited on the sample for TDTR measurements. We observe that in most TDTR measurements, the sensitivity to hAl only depends weakly on the modulation frequency f. Thus, we performed an additional TDTR measurement at a low modulation frequency f0, such that the sensitivity to hAl is comparable but the sensitivity to Λcross is near zero. We then analyze the ratio of the TDTR signals at fh to that at f0, 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.