skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Nanoscale imaging of phonon dynamics by electron microscopy
Abstract Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices 1 , modulation of thermal transport 2 and novel nanostructured thermoelectric materials 3–5 . Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity 2 . There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics.  more » « less
Award ID(s):
2034738 2011967
PAR ID:
10405796
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Nature
Volume:
606
Issue:
7913
ISSN:
0028-0836
Page Range / eLocation ID:
292 to 297
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Plasmonic nanostructures have attracted considerable attention for their ability to couple with light and provide strong electromagnetic energy confinement at subwavelength dimensions. The absorbed portion of the captured electromagnetic energy can lead to significant heating of both the nanostructure and its surroundings, resulting in a rich set of nanoscale thermal processes that defines the subfield of thermoplasmonics with applications ranging from nanochemistry and nanobiology to optoelectronics. Recently, phononic nanostructures have started to attract attention as a platform for manipulation of phonons, enabling control over heat propagation and/or mechanical vibrations. The complex interaction phenomena between photons, electrons, and phonons require appropriate modelling strategies to design nanodevices that simultaneously explore and exploit the optical, thermal, and mechanical degrees of freedom. Examples of such devices are micro‐ and nanoscale opto‐thermo‐mechanical systems for sensing, imaging, energy conversion, and harvesting applications. Here, an overview of the fundamental theory and concepts crucial to the modelling of plasmo‐phonon devices is provided. Particular attention is given to micro‐ and nanoscale modelling frameworks, highlighting their validity ranges and the experimental works that contributed to their validation and led to compelling applications. Finally, an open‐ended outlook focused on emerging applications at the intersection between plasmonics and phononics is presented. 
    more » « less
  2. Abstract As the length scales of materials decrease, the heterogeneities associated with interfaces become almost as important as the surrounding materials. This has led to extensive studies of emergent electronic and magnetic interface properties in superlattices 1–9 . However, the interfacial vibrations that affect the phonon-mediated properties, such as thermal conductivity 10,11 , are measured using macroscopic techniques that lack spatial resolution. Although it is accepted that intrinsic phonons change near boundaries 12,13 , the physical mechanisms and length scales through which interfacial effects influence materials remain unclear. Here we demonstrate the localized vibrational response of interfaces in strontium titanate–calcium titanate superlattices by combining advanced scanning transmission electron microscopy imaging and spectroscopy, density functional theory calculations and ultrafast optical spectroscopy. Structurally diffuse interfaces that bridge the bounding materials are observed and this local structure creates phonon modes that determine the global response of the superlattice once the spacing of the interfaces approaches the phonon spatial extent. Our results provide direct visualization of the progression of the local atomic structure and interface vibrations as they come to determine the vibrational response of an entire superlattice. Direct observation of such local atomic and vibrational phenomena demonstrates that their spatial extent needs to be quantified to understand macroscopic behaviour. Tailoring interfaces, and knowing their local vibrational response, provides a means of pursuing designer solids with emergent infrared and thermal responses. 
    more » « less
  3. Understanding and controlling nonequilibrium electronic phenomena is an outstanding challenge in science and engineering. By electrically driving ultraclean graphene devices out of equilibrium, we observe an instability that is manifested as substantially enhanced current fluctuations and suppressed conductivity at microwave frequencies. Spatial mapping of the nonequilibrium current fluctuations using nanoscale magnetic field sensors reveals that the fluctuations grow exponentially along the direction of carrier flow. Our observations, including the dependence on density and temperature, are consistently explained by the emergence of an electron-phonon Cerenkov instability at supersonic drift velocities. These results offer the opportunity for tunable terahertz generation and active phononic devices based on two-dimensional materials. 
    more » « less
  4. null (Ed.)
    In this work, we report a high thermal conductivity ( k ) of 162 W m −1 K −1 and 52 W m −1 K −1 at room temperature, along the directions perpendicular and parallel to the c -axis, respectively, of bulk hexagonal BC 2 P (h-BC 2 P), using first-principles calculations. We systematically investigate elastic constants, phonon group velocities, phonon linewidths and mode thermal conductivity contributions of transverse acoustic (TA), longitudinal acoustic (LA) and optical phonons. Interestingly, optical phonons are found to make a large contribution of 30.1% to the overall k along a direction perpendicular to the c -axis at 300 K. BC 2 P is also found to exhibit high thermal conductivity at nanometer length scales. At 300 K, a high k value of ∼47 W m −1 K −1 is computed for h-BC 2 P at a nanometer length scale of 50 nm, providing avenues for achieving efficient nanoscale heat transfer. 
    more » « less
  5. Abstract This work explores the 2D interfacial energy transport between monolayer WSe2and SiO2while considering the thermal nonequilibrium between optical and acoustic phonons caused by photoexcitation. Recent modeling and experimental work have shown substantial temperature differences between optical and acoustic phonons (ΔTOA) in various nanostructures upon laser irradiation. Generally, characterizations of interfacial thermal resistance (R′′tc) at the nanoscale are difficult and depend on Raman‐probed temperature measurements, which only reveal optical phonon temperature information. Here it is shown that ΔTOAfor supported monolayer WSe2can be as high as 48% of the total temperature rise revealed by optothermal Raman methods—a significant proportion that can introduce sizeable error toR′′tcmeasurements if not properly considered. A frequency energy transport state‐resolved Raman technique (FET‐Raman) along with a 3D finite volume modeling of 2D material laser heating is used to extract the true interfacial thermal resistanceR′′tc(determined by acoustic phonon transport). Additionally, a novel ET‐Raman technique is developed to determine the energy coupling factorGbetween optical and acoustic phonons (on the order of 1015W m−3K−1). This work demonstrates the need for special consideration of thermal nonequilibriums during laser–matter interactions at the nanoscale. 
    more » « less