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Ruochen Shi

Publications and source records attributed to Ruochen Shi.

At least 19 recordsLinked to original sources

Direct Measurement of Exciton Dispersion in the Long-Wavelength Limit

Exciton dispersion, which governs the propagation, scattering and radiative decay of electron-hole pairs, is essential to optoelectronics and quantum materials. In two-dimensional systems, weakened dielectric screening and long-range electron-hole exchange are predicted to induce nonanalytic exciton dispersion in the long-wavelength limit. However, direct quantitative characterization of its dimensional evolution remains lacking, especially in the ultralow-q regime (q < 0.02 $\r{A}^{-1}$). Here we employ defocus-engineered momentum-resolved electron energy-loss spectroscopy in scanning transmission electron microscopy, achieving an ultrahigh momentum resolution of 0.0002 $\r{A}^{-1}$. Using freestanding hBN as a prototypical platform, we resolve layer-dependent exciton dispersion and quantify its characteristic crossover momentum and group velocity in the long-wavelength limit. With increasing thickness, the nonanalytic linear-dispersion regime is progressively compressed, manifested by a reduction in characteristic crossover momentum q_c from $1.82 \times 10^{-1} \r{A}^{-1}$ in the monolayer to $3.0 \times 10^{-1} \r{A}^{-1}$ in 25 layers. Meanwhile, the low-q group velocity increases from $2.0 \times 10^{-3} c$ to $2.9 \times 10^{-2} c$, before the dispersion ultimately approaches the bulk-like parabolic limit. We further examine how the exciton band structure of monolayer hBN responds to its surrounding environment, including temperature, adjacent graphene layers, and interlayer twist in BN/graphene heterostructures. These findings uncover the fundamental physics of low-dimensional excitons, deliver valuable guidance for modulating exciton transport, diffusion and quasiparticle coupling in layered quantum materials, and establish a powerful experimental route to explore low-dimensional exciton physics.

cond-mat.mes-hall

Nanoscale Thermal Imaging of Dislocation-Mediated Heat Transport

Dislocations in crystalline materials are widely exploited to tailor the thermal conductivity of semiconductors and thermoelectrics, yet a critical gap persists: direct measurement of local thermal resistance at individual buried dislocations, along with its spatial extent, remains elusive due to the limitations of conventional thermal probes. Here, we use in situ scanning transmission electron microscopy-electron energy-loss spectroscopy to map nanoscale temperature distributions across a low-angle SrTiO3 grain boundary with periodic dislocation arrays. Our results reveal a temperature drop of 47 K across the dislocation array. The associated temperature-field distortions are concentrated near the dislocation cores, consistent with stronger local thermal resistance at these discrete sites rather than a uniformly distributed resistance along the array. We further identify a distinct two-scale heat transport characteristic near the dislocation array: core-dominated effects over approximately 4.8-6.2 nm and extended inter-core influences over approximately 10.3-14.3 nm. Atomic-scale structural and vibrational analyses further reveal core-associated atomic reconstruction and localized optical-phonon perturbations, providing a microscopic basis for the stronger local thermal resistance inferred near dislocation cores. These findings quantitatively resolve spatial heterogeneity of dislocation-mediated heat transport, uncover its atomic-scale mechanism, and provide a quantitative basis for defect engineering, guiding the design of high-performance thermoelectrics, semiconductors, high-temperature structural alloys, and other functional crystalline materials.

cond-mat.mtrl-sci

Monolithic integration of diverse crystalline thin films on diamond for near-junction thermal management

The pursuit of extreme miniaturization and high power in 6G RF front-ends has cast thermal dissipation as the central challenge. Here, we have demonstrated the monolithic integration of functionally distinct single-crystal thin films, including \b{eta}-Ga2O3, Si, GaN, and LiTaO3, onto a single diamond substrate using a multi-step transfer printing technique. Focusing on the critical \b{eta}-Ga2O3/diamond interface, we achieve an exceptional interfacial thermal conductance (ITC) of 149 MW m-2 K-1 through ultra-high vacuum (UHV) annealing, creating an atomically sharp interface featuring covalent bonding. Vibrational electron energy-loss spectroscopy (EELS) analysis combining with molecular dynamics (MD) simulations reveal that distinctive interfacial phonon modes at the \b{eta}-Ga2O3/diamond heterointerface dominate ultrahigh ITC. We experimentally demonstrate that by improving the ITC, the thermal resistance (Rth) of a diamond-based \b{eta}-Ga2O3 MOSFET is driven to a record-low value of 1.58 K mm W-1, underscoring the critical role of interface engineering in near-junction thermal management for diamond-integrated devices. This work demonstrates a scalable, diamond-based monolithic integration platform designed to solve the near-junction thermal challenges in high-power RF front-ends.

cond-mat.mtrl-sci

Resolving Phonons in Superconductor Bi2Sr2CaCu2O8+{\delta} at Sub-Unit-Cell Resolution

The role of phonons in cuprates remains controversial, with their complex lattice structure complicating the investigation. Here, we identify phonon modes originating from charge reservoir and superconducting layers of Bi2Sr2CaCu2O8+{\delta} using sub-unit-cell resolved electron energy loss spectroscopy in a scanning transmission electron microscope. We reveal several phonon modes exhibiting layer-specific localization: ~78 meV in-plane modes localized in the CuO2 planes, ~42 meV hybrid (in-plane and out-of-plane) modes in the CuO2 planes, and ~38 meV hybrid modes in the BiO layers. We also observe a periodic modulation of phonon frequencies induced by the superstructure, spatially correlating with the superconducting gap variation. Our findings offer new insights into the electron-phonon coupling in cuprates, fostering deeper exploration of the microscopic linkage between lattice dynamics and superconductivity.

cond-mat.supr-con

Strongly confined Mid-infrared to Terahertz Phonon Polaritons in Ultra-thin SrTiO3

Phonon polaritons (PhPs) enable subwavelength light control for infrared sensing, imaging, and optoelectronics, but conventional polar materials have narrow Reststrahlen bands, limiting applications. Materials that support PhPs with broad spectral range, strong field confinement, slow group velocity, and high quality factor are therefore needed. Here, using monochromatic electron energy loss spectroscopy in a scanning transmission electron microscope, we demonstrate that ultra-thin SrTiO3 membranes possess the desired properties. Systematic measurements across varying thicknesses reveal two PhP branches with wide spectral dispersion, strong confinement, and anomalously slow group velocities spanning from the mid-infrared to terahertz range. Notably, in 3-nm-thick membranes, these polaritons exhibit unprecedented confinement factors exceeding 500 and group velocities as low as ~ 7 x 10-5c, rivaling the best-performing van der Waals materials. These findings establish perovskite oxide such as SrTiO3 as versatile platforms for tailoring light-matter interactions at the nanoscale, providing critical insights for the design of next-generation photonic devices requiring broadband operation and enhanced optical confinement.

physics.optics

Precise structure and polarization determination of Hf0.5Zr0.5O2 with electron ptychography

Hf0.5Zr0.5O2 (HZO) is a promising candidate for next generation ferroelectric memories and transistors. However, its ferroelectricity origin is still under debate due to the complex of its phase and microstructure in practical samples. In this study, we investigate the atomic structure of substrate-free HZO freestanding film with multislice electron ptychography, for which the ultra-high space resolution (up to ~25 pm) and capability to simultaneously image the cation and oxygen allow us to precisely determine the intrinsic atomic structures of different phases and reveal subtle changes among them. We clarify that the orthorhombic phase is ferroelectric with spontaneous polarization ~34{\pm}4 {\mu}C/cm2 (corresponding to 56{\pm}6 pm in displacement) that is accurately measured through statistical analysis. Significant polarization suppression is observed near the grain boundary, while no distinguishable structural changes are detected near the 180{\deg} ferroelectric domain walls. Through the direct oxygen imaging of orthorhombic phase from the [111] zone axis, we quantify a substantial number of oxygen vacancies with a preferential distribution, which influences the polarization direction and strength. These findings provide fundamentals for HZO research, and thus lay a foundation for the design of high-performance ferroelectric devices.

cond-mat.mtrl-sci

Single-atom-resolved vibrational spectroscopy of a dislocation

Phonon resistance from dislocation scattering is often divided into short-range core interactions and long-range strain field interactions. Using electron energy-loss spectroscopy on a GaN dislocation, we report observations of vibrational modes localized at specific core atoms (short-range) and strain-driven phonon energy shifts around the dislocation (long-range). Ab initio calculations support these findings and draw out additional details. This study reveals atomically resolved vibrational spectra of dislocations, thus offering insights for engineering improved material functionalities.

cond-mat.mtrl-sci

Atomic-scale mechanism of enhanced electron-phonon coupling at the interface of MgB$_2$ thin film

In this study, we explore the heterointerface of MgB$_2$ film on SiC substrate at atomic scale using electron microscopy and spectroscopy. We detect ~1 nm MgO between MgB$_2$ and SiC. Atomic-level electron energy loss spectra (EELS) show MgB$_2$-E2g mode splitting and softening near the MgB$_2$/MgO interface. Orbital-resolved core-level EELS link the phonon softening to in-plane boron-atom electron states' changes. Ab initio calculations confirm this softening enhances electron-phonon coupling at the interface. Our findings highlight interface engineering's potential for superconductivity enhancement.

cond-mat.supr-con

Atomically localized ingredient-dependent interface phonon in heterogeneous solids

Phonons are the primary heat carriers in non-metallic solids. In compositionally heterogeneous materials, the thermal properties are believed to be mainly governed by the disrupted phonon transport due to mass disorder and strain fluctuations, while the effects of compositional fluctuation induced local phonon states are usually ignored. Here, by scanning transmission electron microscopy electron energy loss spectroscopy and sophisticated calculations, we identify the vibrational properties of ingredient-dependent interface phonon modes in AlxGa1-xN and quantify their various contributions to the local interface thermal conductance. We demonstrate that atomic-scale compositional fluctuation has significant influence on the vibrational thermodynamic properties, highly affecting the mode ratio and vibrational amplitude of interface phonon modes and subsequently redistributing their modal contribution to the ITC. Our work provides fundamental insights into understanding of local phonon-boundary interactions in nanoscale inhomogeneities, which reveal new opportunities for optimization of thermal properties via engineering ingredient distribution.

cond-mat.mtrl-sci

Phonon transition across an isotopic interface

Natural materials usually consist of isotopic mixtures, for which different isotopic ratios can lead to distinct material properties such as thermal conductivity and nucleation process. However, the knowledge of isotopic interface remains largely unexplored mainly due to the challenges in isotopic identification and property measurement at an atomic scale. Here, by using monochromated electron energy-loss spectroscopy in a scanning transmission electron microscope, we reveal momentum-transfer-dependent lattice vibration behavior at an artificial h-10BN/h-11BN heterostructure with sub-unit-cell resolution. We find the vibrational energy changes across the isotopic interface gradually, featuring a wide transition regime, which suggests strong delocalization of the out-of-plane optical phonons at the interface. In addition, we identify phonons near the Brillouin zone center have a transition regime ~3.34 nm (10 atomic layers), whereas phonons at the Brillouin zone boundary transition in ~1.66 nm (5 atomic layers). We propose that the isotope-induced charge effect at the interface accounts for the distinct delocalization behavior. Moreover, intra-atomic layer variation of vibration energy is also sensitive to the momentum transfer, thus at the interface it depends on both of momentum transfer and mass change. The revealed lattice vibration behavior at an isotopic interface provides new insights to understand the isotopic effects on properties in natural materials.

cond-mat.mtrl-sci

Tunable Interband Transitions in Twisted h-BN/Graphene Heterostructures

In twisted h-BN/graphene heterostructures, the complex electronic properties of the fast-traveling electron gas in graphene are usually considered to be fully revealed. However, the randomly twisted heterostructures may also have unexpected transition behaviors, which may influence the device performance. Here, we study the twist angle-dependent coupling effects of h-BN/graphene heterostructures using monochromatic electron energy loss spectroscopy. We find that the moir\'e potentials alter the band structure of graphene, resulting in a redshift of the intralayer transition at the M-point, which becomes more pronounced up to 0.25 eV with increasing twist angle. Furthermore, the twisting of the Brillouin zone of h-BN relative to the graphene M-point leads to tunable vertical transition energies in the range of 5.1-5.6 eV. Our findings indicate that twist-coupling effects of van der Waals heterostructures should be carefully considered in device fabrications, and the continuously tunable interband transitions through the twist angle can serve as a new degree of freedom to design optoelectrical devices.

cond-mat.mes-hall

Single-dislocation phonons: atomic-scale measurement and their thermal properties

Nanoscale defects such as dislocations, have a significant impact on the phonon thermal transport properties in non-metallic materials. To unravel these effects, understanding of defect phonon modes is essential. Herein, at the atomic scale, the localized phonons of individual dislocation at a Si/Ge interface are measured via monochromated electron energy loss spectroscopy in a scanning transmission electron microscope. These modes are then correlated with the local microstructure, further revealing the dislocation effects on the local thermal transport properties. The dislocation causes phonon redshift in several milli-electron-volts within about two to four nanometers of the core, where both of the strain field and Ge-segregation play roles. With the presence of dislocation, the local interfacial thermal conductance can be either enhanced or reduced, depending on the complex interaction and competition between lattice-disorder (dislocation) and element-disorder (heterointerface mixing and Ge-segregation) at the interface. These findings provide valuable insights to improve the thermal properties of thermoelectric generators and thermal management systems through proper defect engineering.

cond-mat.mtrl-sci

Electron microscopy probing electron-photon interactions in SiC nanowires with ultra-wide energy and momentum match

Nanoscale materials usually can trap light and strongly interact with it leading to many photonic device applications. The light-matter interactions are commonly probed by optical spectroscopy, which, however, have some limitations such as diffraction-limited spatial resolution, tiny momentum transfer and non-continuous excitation/detection. In this work, using scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS) with ultra-wide energy and momentum match and sub-nanometer spatial resolution, we study the optical microcavity resonant spectroscopy in a single SiC nanowire. The longitudinal Fabry-Perot (FP) resonating modes and the transverse whispering-gallery modes (WGMs) are simultaneously excited and detected, which span from near-infrared (~ 1.2 {\mu}m) to ultraviolet (~ 0.2 {\mu}m) spectral regime and the momentum transfer can be ranging up to 108 cm{^{-1}}. The size effects on the resonant spectra of nanowires are also revealed. Moreover, the nanoscale decay length of resonant EELS is revealed, which is contributed by the strongly localized electron-photon interactions in the SiC nanowire. This work provides a new alternative technique to investigate the optical resonating spectroscopy of a single nanowire structure and to explore the light-matter interactions in dielectric nanostructures, which is also promising for modulating free electrons via photonic structures.

cond-mat.mes-hall

Direct observation of local antiferroelectricity induced phonon softening at a SrTiO3 defect

Defects in oxides usually exhibit exotic properties that may be associated with the local lattice dynamics. Here, at atomic spatial resolution, we directly measure phonon modes of an antiphase boundary (APB) in SrTiO3 freestanding membrane and correlate them with the picometer-level structural distortion. We find that the SrTiO3 APB introduces new defect phonon modes that are absent in bulk SrTiO3. These modes are highly sensitive to the subtle structure distortion, i.e., the SrTiO3 APB generates the local electric dipoles forming an antiferroelectric configuration, which significantly softens the transverse optical (TO) and longitudinal optical (LO) modes at {\Gamma} point. Correlating the local phonons with the subtle structural distortion, our findings provide valuable insights into understanding the defect properties in complex oxides and essential information for their applications such as thermoelectric devices.

cond-mat.mtrl-sci

Approaching the Purcell factor limit with whispering-gallery hyperbolic phonon polaritons in hBN nanotubes

Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interaction, thus giving rise to a high density of optical states, as quantified by the so-called Purcell factor - the ratio of the decay rate of an optical quantum emitter to its value in free space. Here, we exploit whispering-gallery hyperbolic-phonon-polariton (WG-HPhP) modes in hBN nanotubes (BNNTs) to demonstrate record-high Purcell factors (~10^12) driven by the deep-subwavelength confinement of phonon polaritons and the low intrinsic losses in these atomically smooth nanocavities. Furthermore, the measured Purcell factor increases with decreasing BNNT radius down to 5 nm, a result that extrapolates to ~10^14 in a single-walled BNNT. Our study supports WG-HPhP modes in one-dimensional nanotubes as a powerful platform for investigating ultrastrong light-matter interactions, which open exciting perspectives for applications in single-molecular sensors and nanolasers.

physics.optics

Electric-field control of the nucleation and motion of isolated three-fold polar vertices

Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO3/SrRuO3 interface, a two-unit-cell thick SrTiO3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s-1. Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.

cond-mat.mtrl-sci

Measuring phonon dispersion at an interface

The breakdown of translational symmetry at heterointerfaces leads to the emergence of new phonon modes localized near the interface. These interface phonons play an essential role in thermal/electrical transport properties in devices especially in miniature ones wherein the interface may dominate the entire response of the device. Knowledge of phonon dispersion at interfaces is therefore highly desirable for device design and optimization. Although theoretical work has begun decades ago, experimental research is totally absent due to challenges in achieving combined spatial, momentum and spectral resolutions required to probe localized phonon modes. Here we use electron energy loss spectroscopy in an electron microscope to directly measure both the local phonon density of states and the interface phonon dispersion relation for an epitaxial cBN-diamond heterointerface. In addition to bulk phonon modes, we observe acoustic and optical phonon modes localized at the interface, and modes isolated away from the interface. These features only appear within ~ 1 nm around the interface. The experimental results can be nicely reproduced by ab initio calculations. Our findings provide insights into lattice dynamics at heterointerfaces and should be practically useful in thermal/electrical engineering.

cond-mat.mtrl-sci

Four-dimensional Vibrational Spectroscopy for Nanoscale Mapping of Phonon Dispersion in BN Nanotubes

Direct measurement of local phonon dispersion in individual nanostructures can greatly advance our understanding of their electrical, thermal, and mechanical properties. However, such experimental measurements require extremely high detection sensitivity and combined spatial, energy and momentum resolutions, thus has been elusive. Here, we develop a four-dimensional electron energy loss spectroscopy (4D-EELS) technique based a monochromated scanning transmission electron microscope (STEM), and present the position-dependent phonon dispersion measurement in individual boron nitride nanotubes (BNNTs). Our measurement shows that the unfolded phonon dispersion of multi-walled BNNTs is close to hexagonal-boron nitride (h-BN) crystals, suggesting that interlayer coupling and curved geometry have no substantial impacts on phonon dispersion. We also find that the acoustic phonons are extremely sensitive to momentum-dependent defect scattering, while optical phonons are much less susceptible. This work not only provides useful insights into vibrational properties of BNNTs, but also demonstrates huge prospects of the developed 4D-EELS technique in nanoscale phonon dispersion measurements.

cond-mat.mes-hall