skip to main content

Attention:

The NSF Public Access Repository (NSF-PAR) system and access will be unavailable from 11:00 PM ET on Thursday, October 10 until 2:00 AM ET on Friday, October 11 due to maintenance. We apologize for the inconvenience.


Title: Visualizing Energy Transfer at Buried Interfaces in Layered Materials Using Picosecond X‐Rays
Abstract

Understanding the fundamentals of nanoscale heat propagation is crucial for next‐generation electronics. For instance, weak van der Waals bonds of layered materials are known to limit their thermal boundary conductance (TBC), presenting a heat dissipation bottleneck. Here, a new nondestructive method is presented to probe heat transport in nanoscale crystalline materials using time‐resolved X‐ray measurements of photoinduced thermal strain. This technique directly monitors time‐dependent temperature changes in the crystal and the subsequent relaxation across buried interfaces by measuring changes in thec‐axis lattice spacing after optical excitation. Films of five different layered transition metal dichalcogenides MoX2[X = S, Se, and Te] and WX2[X = S and Se] as well as graphite and a W‐doped alloy of MoTe2are investigated. TBC values in the range 10–30 MW m−2K−1are found, onc‐plane sapphire substrates at room temperature. In conjunction with molecular dynamics simulations, it is shown that the high thermal resistances are a consequence of weak interfacial van der Waals bonding and low phonon irradiance. This work paves the way for an improved understanding of thermal bottlenecks in emerging 3D heterogeneously integrated technologies.

 
more » « less
NSF-PAR ID:
10363674
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Functional Materials
Volume:
30
Issue:
34
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Van der Waals interactions in 2D materials have enabled the realization of nanoelectronics with high‐density vertical integration. Yet, poor energy transport through such 2D–2D and 2D–3D interfaces can limit a device's performance due to overheating. One long‐standing question in the field is how different encapsulating layers (e.g., contact metals or gate oxides) contribute to the thermal transport at the interface of 2D materials with their 3D substrates. Here, a novel self‐heating/self‐sensing electrical thermometry platform is developed based on atomically thin, metallic Ti3C2MXene sheets, which enables experimental investigation of the thermal transport at a Ti3C2/SiO2interface, with and without an aluminum oxide (AlOx) encapsulating layer. It is found that at room temperature, the thermal boundary conductance (TBC) increases from 10.8 to 19.5 MW m−2K−1upon AlOxencapsulation. Boltzmann transport modeling reveals that the TBC can be understood as a series combination of an external resistance between the MXene and the substrate, due to the coupling of low‐frequency flexural acoustic (ZA) phonons to substrate modes, and an internal resistance between ZA and in‐plane phonon modes. It is revealed that internal resistance is a bottle‐neck to heat removal and that encapsulation speeds up the heat transfer into low‐frequency ZA modes and reduces their depopulation, thus increasing the effective TBC.

     
    more » « less
  2. Abstract

    Heat transport across vertical interfaces of heterogeneous 2D materials is usually governed by the weak Van der Waals interactions of the surface‐terminating atoms. Such interactions play a significant role in thermal transport across transition metal carbide and nitride (MXene) atomic layers due to their hydrophilic nature and variations in surface terminations. Here, the metallicity of atomically thin Ti3C2TzMXene, which is also verified by scanning tunneling spectroscopy for the first time, is exploited to develop a self‐heating/self‐sensing platform to carry out direct‐current annealing experiments in high (<10−8bar) vacuum, while simultaneously evaluating the interfacial heat transport across a Ti3C2Tz/SiO2interface. At room temperature, the thermal boundary conductance (TBC) of this interface is found, on average, to increase from 10 to 27 MW m−2K−1upon current annealing up to the breakdown limit. In situ heating X‐ray diffraction and X‐ray photo‐electron spectroscopy reveal that the TBC values are mainly affected by interlayer and interface spacing due to the removal of absorbents, while the effect of surface termination is negligible. This study provides key insights into understanding energy transport in MXene nanostructures and other 2D material systems.

     
    more » « less
  3. Abstract

    The transition metal selenides M1+ySe2(M = V, Ti) have intriguing quantum properties, which make them target materials for controlling properties by thinning them to the ultrathin limit. An appropriate approach for the synthesis of such ultrathin films is by molecular beam epitaxy. Here, it is shown that such synthesized V‐ and Ti‐Se2films can undergo a compositional change by vacuum annealing. Combined scanning tunneling and photoemission spectroscopy is used to determine compositional and structural changes of ultrathin films as a function of annealing temperature. Loss of selenium from the film is accompanied by a morphology change of monolayer height islands to predominantly bilayer height. In addition, crystal periodicity and atomic structure changes are observed. These changes are consistent with a transition from a layered transition metal dichalcogenide (TMDC) to ordered intercalation compounds with V or Ti intercalated in between two layers of their respective TMDCs. These observations may clear up misconception of the nature of previously reported high‐temperature grown transition metal selenides. More significantly, the demonstrated control of the formation of intercalation compounds is a key step toward modifying properties in van der Waals systems and toward expanding material systems for van der Waals heterostructures.

     
    more » « less
  4. Abstract

    Emergent color centers with accessible spins hosted by van der Waals materials have attracted substantial interest in recent years due to their significant potential for implementing transformative quantum sensing technologies. Hexagonal boron nitride (hBN) is naturally relevant in this context due to its remarkable ease of integration into devices consisting of low-dimensional materials. Taking advantage of boron vacancy spin defects in hBN, we report nanoscale quantum imaging of low-dimensional ferromagnetism sustained in Fe3GeTe2/hBN van der Waals heterostructures. Exploiting spin relaxometry methods, we have further observed spatially varying magnetic fluctuations in the exfoliated Fe3GeTe2flake, whose magnitude reaches a peak value around the Curie temperature. Our results demonstrate the capability of spin defects in hBN of investigating local magnetic properties of layered materials in an accessible and precise way, which can be extended readily to a broad range of miniaturized van der Waals heterostructure systems.

     
    more » « less
  5. Abstract

    Interfacial adhesion energy is a fundamental property of two-dimensional (2D) layered materials and van der Waals heterostructures due to their intrinsic ultrahigh surface to volume ratio, making adhesion forces very strong in many processes related to fabrication, integration and performance of devices incorporating 2D crystals. However, direct quantitative characterization of adhesion behavior of fresh and aged homo/heterointerfaces at nanoscale has remained elusive. Here, we use an atomic force microscopy technique to report precise adhesion measurements in ambient air through well-defined interactions of tip-attached 2D crystal nanomesas with 2D crystal and SiOxsubstrates. We quantify how different levels of short-range dispersive and long-range electrostatic interactions respond to airborne contaminants and humidity upon thermal annealing. We show that a simple but very effective precooling treatment can protect 2D crystal substrates against the airborne contaminants and thus boost the adhesion level at the interface of similar and dissimilar van der Waals heterostructures. Our combined experimental and computational analysis also reveals a distinctive interfacial behavior in transition metal dichalcogenides and graphite/SiOxheterostructures beyond the widely accepted van der Waals interaction.

     
    more » « less