Probing nanoscale thermal transport with cathodoluminescence thermometry
Kelly W. Mauser, Magdalena Solà-Garcia, Matthias Liebtrau, Benjamin Damilano, Pierre-Marie Coulon, Stéphane Vézian, Philip Shields, Sophie Meuret, Albert Polman
Thermal properties have an outsized impact on efficiency and sensitivity of devices with nanoscale structures, such as in integrated electronic circuits. A number of thermal conductivity measurements for semiconductor nanostructures exist, but are hindered by the diffraction limit of light, the need for transducer layers, the slow-scan rate of probes, ultra-thin sample requirements, or extensive fabrication. Here, we overcome these limitations by extracting temperature from measurements of bandgap cathodoluminescence in GaN nanowires with spatial resolution limited by the electron cascade, and use this to determine thermal conductivities in the range of 19-68 W/m*K in three new ways. The electron beam acts simultaneously as a temperature probe and as a controlled delta-function-like heat source to measure thermal conductivities using steady-state methods, and we introduce a frequency-domain method using pulsed electron beam excitation. The different thermal conductivity measurements we explore agree within error where comparable. Our results provide novel methods of measuring thermal properties that allow for rapid, in-situ, high-resolution measurements of integrated circuits and semiconductor nanodevices, and open the door for electron-beam based nanoscale phonon transport studies.
Crucial to analyze phenomena as varied as plasmonic hot spots and the spread of cancer in living tissue, nanoscale thermometry is challenging: probes are usually larger than the sample under study, and contact techniques may alter the sample temperature itself. Many photostable nanomaterials whose luminescence is temperature-dependent, such as lanthanide-doped phosphors, have been shown to be good non-contact thermometric sensors when optically excited. Using such nanomaterials, in this work we accomplished the key milestone of enabling far-field thermometry with a spatial resolution that is n…
The microelectronics industry is pushing the fundamental limit on the physical size of individual elements to produce faster and more powerful integrated chips. These chips have nanoscale features that dissipate power resulting in nanoscale hotspots leading to device failures. To understand the reliability impact of the hotspots, the device needs to be tested under the actual operating conditions. Therefore, the development of high-resolution thermometry techniques is required to understand the heat dissipation processes during the device operation. Recently, several thermometry techniques hav…
The impulsive excitation of ensembles of excitons or color centers by a high-energy electron beam results in the observation of photon bunching in the second-order correlation function of the cathodoluminescence generated by those emitters. Photon bunching in cathodoluminescence microscopy can be used to resolve the excited-state dynamics and the excitation and emission efficiency of nanoscale materials, and it can be used to probe interactions between emitters and nanophotonic cavities. Here, we report substantial changes in the measured bunching induced by indirect electron interactions (wit…
Following the lifespan of optical excitations from their creation to decay into photons is crucial in understanding materials optical properties. Macroscopically, techniques such as the photoluminescence excitation spectroscopy provide unique information on the photophysics of materials with applications as diverse as quantum optics or photovoltaics. Materials excitation and emission pathways are affected by nanometer scale variations directly impacting devices performances. However, they cannot be directly accessed, despite techniques, such as optical spectroscopies with free electrons, havin…
We use simultaneous electronic transport and optical characterization measurements to reveal new information about electronic and optical processes in nanoscale junctions fabricated by electromigration. Comparing electronic tunneling and photocurrents allows us to infer the optical frequency potential difference produced by the plasmon response of the junction. Together with the measured tunneling conductance, we can then determine the locally enhanced electric field within the junction. In similar structures containing molecules, anti-Stokes and Stokes Raman emission allow us to infer the eff…
We demonstrate an all-optical thermometer based on an ensemble of silicon-vacancy centers (SiVs) in diamond by utilizing a temperature dependent shift of the SiV optical zero-phonon line transition frequency, $Δλ/ΔT= 6.8\,\mathrm{GHz/K}$. Using SiVs in bulk diamond, we achieve $70\,\mathrm{mK}$ precision at room temperature with a sensitivity of $360\,\mathrm{mK/\sqrt{Hz}}$. Finally, we use SiVs in $200\,\mathrm{nm}$ nanodiamonds as local temperature probes with $521\,\mathrm{ mK/\sqrt{Hz}}$ sensitivity. These results open up new possibilities for nanoscale thermometry in biology, chemistry, a…
Versatile nanoscale sensors that are susceptible to changes in a variety of physical quantities often exhibit limited selectivity. This paper reports a novel scheme based on microwave-dressed spin states for optically probed nanoscale temperature detection using diamond quantum sensors, which provides selective sensitivity to temperature changes. By combining this scheme with a continuous pump-probe scheme using ensemble nitrogen-vacancy centers in nanodiamonds, a sub-microsecond temporal resolution with thermal sensitivity of 3.7 K$\cdot$Hz$^{-1/2}$ that is insensitive to variations in extern…
The operation of resistive and phase-change memory (RRAM and PCM) is controlled by highly localized self-heating effects, yet detailed studies of their temperature are rare due to challenges of nanoscale thermometry. Here we show that the combination of Raman thermometry and scanning thermal microscopy (SThM) can enable such measurements with high spatial resolution. We report temperature-dependent Raman spectra of HfO$_2$, TiO$_2$ and Ge$_2$Sb$_2$Te$_5$ (GST) films, and demonstrate direct measurements of temperature profiles in lateral PCM devices. Our measurements reveal that electrical and …
Understanding the coordination of cell division timing is one of the outstanding questions in the field of developmental biology. One active control parameter of the cell cycle duration is temperature, as it can accelerate or decelerate the rate of biochemical reactions. However, controlled experiments at the cellular-scale are challenging due to the limited availability of biocompatible temperature sensors as well as the lack of practical methods to systematically control local temperatures and cellular dynamics. Here, we demonstrate a method to probe and control the cell division timing in C…
Temperature imaging of nanoscale systems is a fundamental problem which has myriad potential technological applications. For example, nanoscopic cold spots can be used for spot cooling electronic components while hot spots could be used for precise activation of chemical or biological reactions. More fundamentally, imaging the temperature fields in quantum coherent conductors can provide a wealth of information on heat flow and dissipation at the smallest scales. However, despite significant technological advances, the spatial resolution of temperature imaging remains in the few nanometers ran…
The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS$_2$ with AlN and SiO$_2$, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ~ 15 MWm$^-$$^2$K$^-$$^1$ near room temperature, increasing as ~ T$^0$$^.$$^6$$^5$ in the range 300 -…
We develop a high frequency, wide bandwidth radiometer operating at room temperature, which augments the traditional technique of Johnson noise thermometry for nanoscale thermal transport studies. Employing low noise amplifiers and an analog multiplier operating at 2~GHz, auto- and cross-correlated Johnson noise measurements are performed in the temperature range of 3 to 300~K, achieving a sensitivity of 5.5~mK (110 ppm) in 1 second of integration time. This setup allows us to measure the thermal conductance of a boron nitride encapsulated monolayer graphene device over a wide temperature rang…
Revealing time characteristics of optical excitations in dielectric and plasmonic structures through cathodoluminescence interferometry
NWO-Institute AMOLF（荷兰皇家艺术与科学学院AMOLF研究所）；Kobe University（神户大学）；Universitat Rovira i Virgili（罗维拉-伊-维尔吉利大学）；ICREA-Institució Catalana de Recerca i Estudis Avançats（加泰罗尼亚研究与高等研究院）；ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（巴塞罗那科技研究所光子科学研究所）
Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential impact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source br…
We analyze the benefits and shortcomings of a thermal control in nanoscale electronic conductors by means of the contact heating scheme. Ideally, this straightforward approach allows one to apply a known thermal bias across nanostructures directly through metallic leads, avoiding conventional substrate intermediation. We show, by using the average noise thermometry and local noise sensing technique in InAs nanowire based devices, that a nanoscale metallic constriction on a SiO2 substrate acts like a diffusive conductor with negligible electron-phonon relaxation and non-ideal leads. The non-uni…
Structural, electronic, and chemical nanoscale modifications of transition metal dichalcogenide monolayers alter their optical properties, including the generation of single photon emitters. A key missing element for complete control is a direct spatial correlation of optical response to nanoscale modifications, due to the large gap in spatial resolution between optical spectroscopy and nanometer resolved techniques, such as transmission electron microscopy or scanning tunneling microscopy. Here, we bridge this gap by obtaining nanometer resolved optical properties using electron spectroscopy,…
We present a method for nanoscale thermal imaging of insulating thin films using atomic force microscopy (AFM), and we demonstrate its utility on VO$_2$. We sweep the applied voltage $V$ to a conducting AFM tip in contact mode and measure the local current $I$ through the film. By fitting the $IV$ curves to a Poole-Frenkel conduction model at low $V$, we calculate the local temperature with spatial resolution better than 50 nm using only fundamental constants and known film properties. Our thermometry technique enables local temperature measurement of \textit{any} insulating film dominated by …
Energy dissipation is a fundamental process governing the dynamics of physical, chemical, and biological systems. It is also one of the main characteristics distinguishing quantum and classical phenomena. In condensed matter physics, in particular, scattering mechanisms, loss of quantum information, or breakdown of topological protection are deeply rooted in the intricate details of how and where the dissipation occurs. Despite its vital importance the microscopic behavior of a system is usually not formulated in terms of dissipation because the latter is not a readily measureable quantity on …
Temperature is a fundamental parameter in the study of physical phenomena. At the nanoscale, local temperature differences can be harnessed to design novel thermal nanoelectronic devices or test quantum thermodynamical concepts. Determining temperature locally is hence of particular relevance. Here, we present a primary electron thermometer that allows probing the local temperature of a single electron reservoir in single-electron devices. The thermometer is based on cyclic electron tunneling between a system with discrete energy levels and a single electron reservoir. When driven at a finite …
Mapping the thermal transport properties of materials at the nanoscale is of critical importance for optimizing heat conduction in nanoscale devices. Several methods to determine the thermal conductivity of materials have been developed, most of them yielding an average value across the sample, thereby disregarding the role of local variations. Here, we present a method for the spatially-resolved assessment of the thermal conductivity of suspended graphene by using a combination of confocal Raman thermometry and a finite-element calculations-based fitting procedure. We demonstrate the working …
The advancement of nanoscale electronics has been limited by energy dissipation challenges for over a decade. Such limitations could be particularly severe for two-dimensional (2D) semiconductors integrated with flexible substrates or multi-layered processors, both being critical thermal bottlenecks. To shed light into fundamental aspects of this problem, here we report the first direct measurement of spatially resolved temperature in functioning 2D monolayer MoS$_2$ transistors. Using Raman thermometry we simultaneously obtain temperature maps of the device channel and its substrate. This dif…
Gallium nitride (GaN) is a typical wide-bandgap semiconductor with a critical role in a wide range of electronic applications. Ballistic thermal transport at nanoscale hotspots will greatly reduce the performance of a device when its characteristic length reaches the nanometer scale, due to heat dissipation. In this work, we developed a tip-enhanced Raman thermometry approach to study ballistic thermal transport within the range of 10 nm in GaN, simultaneously achieving laser heating and measuring the local temperature. The Raman results showed that the temperature increase from an Au-coated t…
In ballistic transport, heat carriers such as phonons travel through the solid without any scattering or interaction. Therefore, there is no temperature gradient in the solid, which seems to transport the heat without getting heated itself. Ballistic transport is typically seen in high purity crystals at either temperatures below ~10 K, or physical size below ~100 nm, where the mean free path of the carrier is larger than the solid itself. In this letter, we show evidence of ballistic transport at room temperature in lithium niobate wafers in the in-plane and cross-plane directions under both …
The design and fabrication of phononic crystals (PnCs) hold the key to control the propagation of heat and sound at the nanoscale. However, there is a lack of experimental studies addressing the impact of order/disorder on the phononic properties of PnCs. Here, we present a comparative investigation of the influence of disorder on the hypersonic and thermal properties of two-dimensional PnCs. PnCs of ordered and disordered lattices are fabricated of circular holes with equal filling fractions in free-standing Si membranes. Ultrafast pump and probe spectroscopy (asynchronous optical sampling) a…
