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1. Thermal Transport through CTAB- and MTAB-Functionalized Gold Interfaces Using Molecular Dynamics Simulations

   https://doi.org/10.1021/acs.jcim.4c02195  

   Shavalier, Sydney A; Gezelter, J Daniel (January 2025, Journal of Chemical Information and Modeling)

   Thermal transport coefficients, notably the interfacial thermal conductance, were determined in planar and spherical gold interfaces functionalized with CTAB (cetyltrimethylammonium bromide) or MTAB (16-mercapto-hexadecyl-trimethylammonium bromide) using reverse non-equilibrium molecular dynamics (RNEMD) methods. The systems of interest included (111), (110), and (100) planar facets as well as nanospheres (r = 10 Å). The effect of metal polarizability was investigated through the implementation of the density-readjusted embedded atom model (DR-EAM), a polarizable metal potential. We find that conductance is higher in MTAB-capped interfaces, due in large part to the metal-to-ligand coupling provided by the Au-S bond. Alternatively, CTAB does not couple strongly with either the metal or the solvent, and it is largely a barrier to heat transfer, resulting in a much lower interfacial thermal conductance. Through analysis of physical contact between the ligand and the solvent, we find that there is significantly more overlap in the MTAB systems than the CTAB systems, mirroring the trends we observed in the conductance. 

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2. Thermal Transport in Citrate-Capped Gold Interfaces Using a Polarizable Force Field

   https://doi.org/10.1021/acs.jpcc.2c01333  

   Shavalier, Sydney A.; Gezelter, J. Daniel (January 2022, The Journal of Physical Chemistry C)

   The interfacial thermal conductance from solvated gold nanostructures capped with sodium citrate was determined using reverse nonequilibrium molecular dynamics (RNEMD) methods. The surfaces of spherical nanoparticles and the (111) surfaces of fcc gold slabs were modeled using the density readjusting-embedded atom method (DR-EAM) as well as with the standard embedded atom method (EAM), and the effects of polarizability on the binding preferences of citrate were determined. We find that the binding configurations of citrate depend significantly on gold surface curvature and are not strongly influenced by surface polarizability. The interfacial thermal conductance was also determined for the spherical nanoparticles and (111) surfaces, and we find that applying DR-EAM increases the interfacial thermal conductance for systems with spherical nanoparticles much more sharply than for systems with (111) surfaces. Through analysis of excess charge density near the interface, we find that inclusion of polarizability has a larger impact on image charge creation in nanospheres than it does for the planar (111) interfaces. This effectively increases the interaction strength to polar species in the solvent, yielding larger interfacial thermal conductance estimates for the nanospheres. 

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3. A review of heat transport in solvated gold nanoparticles: Molecular dynamics modeling and experimental perspectives

   https://doi.org/10.1039/D5NR02521D  

   Munshi, Md_Adnan Mahathir; Chowdhury, Emdadul Haque; Paniagua-Guerra, Luis E; Dionne, Jaymes; Giri, Ashutosh; Ramos-Alvarado, Bladimir (September 2025, Nanoscale)

   Turning gold nanoparticles (AuNPs) into nanoscale heat sources via light irradiation has prompted significant research interest, particularly for biomedical applications, over the past few decades. The AuNP’s tunable photothermal effect, notable biocompatibility, and ability to serve as vehicles for temperature-sensitive chemical linkers enable thermo-therapeutics, such as localized drug/gene delivery and thermal ablation of cancerous tissue. Thermal transport in aqueous AuNP solutions stands as the fundamental challenge to developing targeted thermal therapies; thus, this review article surveys recent advancements in our understanding of heat transfer and surface chemistry in AuNPs, with a particular focus on thermal boundary conductance across gold- and functionalized-gold-water interfaces. This review article highlights computational advances based on molecular dynamics simulations that offer valuable insights into nanoscopic interfacial heat transfer in solvated interfaces, particularly for chemically functionalized AuNPs. Additionally, it outlines current experimental techniques for measuring interfacial thermal transport, their limitations, and potential pathways to improve sensitivity. This review further examines computational methodologies to guide the accurate modeling of solvated gold interfaces. Finally, it concludes with a discussion of future research directions aimed at deepening our understanding of interfacial heat transfer in solvated AuNPs, crucial to optimize thermoplasmonic applications. 

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4. Ultra‐High Interfacial Thermal Conductance via Double hBN Encapsulation for Efficient Thermal Management of 2D Electronics

   https://doi.org/10.1002/smll.202205726  

   Ye, Fan; Liu, Qingchang; Xu, Baoxing; Feng, Philip X. ‐L.; Zhang, Xian (February 2023, Small)

   Abstract Heat dissipation is a major limitation of high‐performance electronics. This is especially important in emerging nanoelectronic devices consisting of ultra‐thin layers, heterostructures, and interfaces, where enhancement in thermal transport is highly desired. Here, ultra‐high interfacial thermal conductance in encapsulated van der Waals (vdW) heterostructures with single‐layer transition metal dichalcogenides MX₂(MoS₂, WSe₂, WS₂) sandwiched between two hexagonal boron nitride (hBN) layers is reported. Through Raman spectroscopic measurements of suspended and substrate‐supported hBN/MX₂/hBN heterostructures with varying laser power and temperature, the out‐of‐plane interfacial thermal conductance in the vertical stack is calibrated. The measured interfacial thermal conductance between MX₂and hBN reaches 74 ± 25 MW m⁻²K⁻¹, which is at least ten times higher than the interfacial thermal conductance of MX₂in non‐encapsulation structures. Molecular dynamics (MD) calculations verify and explain the experimental results, suggesting a full encapsulation by hBN layers is accounting for the high interfacial conductance. This ultra‐high interfacial thermal conductance is attributed to the double heat transfer pathways and the clean and tight vdW interface between two crystalline 2D materials. The findings in this study reveal new thermal transport mechanisms in hBN/MX₂/hBN structures and shed light on building novel hBN‐encapsulated nanoelectronic devices with enhanced thermal management. 

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5. Effect of light atoms on thermal transport across solid–solid interfaces

   https://doi.org/10.1039/C9CP03426A  

   Li, Ruiyang; Gordiz, Kiarash; Henry, Asegun; Hopkins, Patrick E.; Lee, Eungkyu; Luo, Tengfei (August 2019, Physical Chemistry Chemical Physics)

   Thermal transport across solid interfaces is of great importance for applications like power electronics. In this work, we perform non-equilibrium molecular dynamics simulations to study the effect of light atoms on the thermal transport across SiC/GaN interfaces, where light atoms refer to substitutional or interstitial defect atoms lighter than those in the pristine lattice. Various light atom doping features, such as the light atom concentration, mass of the light atom, and skin depth of the doped region, have been investigated. It is found that substituting Ga atoms in the GaN lattice with lighter atoms ( e.g. boron atoms) with 50% concentration near the interface can increase the thermal boundary conductance (TBC) by up to 50%. If light atoms are introduced interstitially, a similar increase in TBC is observed. Spectral analysis of interfacial heat transfer reveals that the enhanced TBC can be attributed to the stronger coupling of mid- and high-frequency phonons after introducing light atoms. We have also further included quantum correction, which reduces the amount of enhancement, but it still exists. These results may provide a route to improve TBC across solid interfaces as light atoms can be introduced during material growth. 

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