arXiv subjects

Aleksandra Radenovic

Publications and source records attributed to Aleksandra Radenovic.

At least 19 recordsLinked to original sources

arXiv2026

In-situ correlative SEM/KPFM for semiconductor devices and 2D heterostructures

Correlative nanoscale surface characterization benefits from simultaneously measuring electronic and structural properties in the same environment, a capability that is essential for modern-day materials science and semiconductor failure analysis. In-situ AFM-SEM measurements facilitated by self-sensing cantilevers offer great potential here; however, they are limited due to their inherent capacitive crosstalk. Here, we demonstrate for the first time the in-situ implementation of single-pass heterodyne Kelvin probe force microscopy inside a scanning electron microscope, using piezo-resistive cantilevers. We overcome the capacitive crosstalk prevalent in piezo-resistive cantilevers by demodulating excitation and detection to simultaneously map surface topography and contact potential difference for correlation with compositional analysis. We systematically compare different operational modes of this heterodyne technique, elucidating their spatial resolution, signal sensitivity, and signal-to-noise ratio. The integrated approach yields exceptional signal quality and reveals how electron beam scan parameters can directly influence surface potential contrast. We demonstrate this correlative analysis workflow on two-dimensional heterostructures and semiconductor circuits. This work establishes a robust and versatile correlative imaging mode for in-situ Kelvin force and topography imaging inside a scanning electron microscope for next-generation semiconductor device analysis and materials science.

cond-mat.mes-hall↗

arXiv2026

Energy-Transfer-Enhanced Emission and Quantum Sensing of VB- Defects in hBN-PbI2 Heterostructures

Spin defects in two-dimensional materials hold significant potential for quantum information technologies and sensing applications. The negatively charged boron vacancy (VB-) in hexagonal boron nitride (hBN) has attracted considerable attention as a quantum sensor due to its demonstrated sensitivity to temperature, magnetic fields, and pressure.1 However, its applications have thus far been limited by inherently dim photoluminescence (PL). By fabricating a van der Waals heterostructure with a sensitizing donor layer, lead iodide (PbI2), we effectively enhance the PL intensity from the VB- by 5-45x, while maintaining compatibility with other heterostructures and vdW optoelectronic platforms. The type-I band alignment at the heterojunction enables efficient exciton migration while suppressing back-electron transfer, and the strong spectral overlap between the PbI2 emission and defect absorption supports efficient fluorescence resonance energy transfer. Ab initio density functional theory (DFT) predicts a photon-ratcheting mechanism that boosts absorption and emission while maintaining magnetic resonance (ODMR) contrast through minimal hybridization. Experimentally, the heterostructure exhibits enhanced continuous-wave ODMR sensitivity and functions as a precise probe of external magnetic fields. This work establishes a proof-of-concept for amplifying weak defect signals in nanomaterials, highlighting a new strategy for engineering their optical and magnetic responses.

cond-mat.mtrl-sci↗

arXiv2025

Direct imaging elucidates ionic memory in two-dimensional nanochannels

Nanofluidic memristors promise brain-inspired information processing with ions, yet their microscopic origin remains debated. So far, ionic memory has been attributed to ion-specific interactions, dynamic wetting, chemical reactions or mechanical deformations, yet typically without direct experimental evidence. Here, by combining operando interferometric imaging with electrokinetic measurements, we directly visualize voltage-induced blistering of the confining walls of two-dimensional (2D) nanochannels, as key origin of memristive hysteresis. We identify two distinct classes of blisters: unidirectional, driven by electrostatic forces on surface charges, and bidirectional, arising from osmotic pressure due to concentration polarization. This mechanistic framework explains device evolution and device-to-device variability, and reframes stochastic blistering as a functional design element. Our results constitute a direct proof of electromechanical coupling as a robust pathway to ionic memory in 2D nanochannels and open routes toward high-performance ionic memristors and electrically actuated nanofluidic valves.

cond-mat.mes-hall↗

arXiv2025

Isotopic Fingerprints of Proton-mediated Dielectric Relaxation in Solid and Liquid Water

We report cross-validated measurements of the isotope effect on dielectric relaxation for four isotopologues of ice and water, including the 1-10^5 Hz region, in which only sporadic and inconsistent measurements were previously available. In ice, the relaxation rates exhibit an activated temperature dependence with an isotope-independent activation energy. Across 248-273 K, the H_2O/D_2O relaxation rate ratio remains constant at 2.0 \pm 0.1. This scaling agrees with Kramers' theory in the high-friction limit if the moving mass is the proton or deuteron, indicating that dielectric relaxation is governed by a classic proton transfer over an energy barrier rather than molecular reorientation.

physics.chem-ph↗

arXiv2024

Could ChatGPT get an Engineering Degree? Evaluating Higher Education Vulnerability to AI Assistants

AI assistants are being increasingly used by students enrolled in higher education institutions. While these tools provide opportunities for improved teaching and education, they also pose significant challenges for assessment and learning outcomes. We conceptualize these challenges through the lens of vulnerability, the potential for university assessments and learning outcomes to be impacted by student use of generative AI. We investigate the potential scale of this vulnerability by measuring the degree to which AI assistants can complete assessment questions in standard university-level STEM courses. Specifically, we compile a novel dataset of textual assessment questions from 50 courses at EPFL and evaluate whether two AI assistants, GPT-3.5 and GPT-4 can adequately answer these questions. We use eight prompting strategies to produce responses and find that GPT-4 answers an average of 65.8% of questions correctly, and can even produce the correct answer across at least one prompting strategy for 85.1% of questions. When grouping courses in our dataset by degree program, these systems already pass non-project assessments of large numbers of core courses in various degree programs, posing risks to higher education accreditation that will be amplified as these models improve. Our results call for revising program-level assessment design in higher education in light of advances in generative AI.

cs.CY↗

arXiv2024

All-water supercapacitor enabled by 1-nm clay channels

Water confined to channels one nanometer thick exhibits electrochemical behavior distinct from bulk water, including enhanced protonic conductivity and large dielectric anisotropy. Here, we exploit these characteristics to design a scalable electrochemical energy-storage system ("blue capacitor") constructed entirely from naturally abundant materials. By assembling layered clays and conductive graphene, we produce 1-nm-thick channels in which confined water acts as the sole electrolyte. We systematically study different clay types, the electrode composition, and separator thickness using complementary physicochemical and electrochemical techniques. The device operates stably up to 1.6 V, achieves specific capacitances of up to 40 F/g, nearly 100% coulombic efficiency, and stable performance over more than 60,000 charge-discharge cycles. Structural and dynamic analyses validate the device architecture, water purity, and proton transport in the nanopores. These results demonstrate that nanoconfined water can function as an electrolyte in a macroscopic electrochemical device, providing a platform for exploring sustainable aqueous energy-storage systems.

cond-mat.soft↗

arXiv2024

Emission dipole orientation reveals dynamic single-molecule interactions with 2D crystals at solvent interfaces

Direct observation of individual fluorescent emitters is crucial for understanding and studying quantum materials, chemical reactions, and biological systems. However, current single-molecule tracking methods only focuses on the localizations of molecules, overlooking molecular configuration and orientation. In this work, we introduce a high-throughput polarized single-molecule localization microscopy that simultaneously resolves the locations and emission dipole orientations of single fluorescent emitters with nanometer precision. Using the interface between pristine hexagonal boron nitride (h-BN) and an organic solvent as a challenging platform, we capture over 10^5 fluorescent events and reveal distinct molecular interaction dynamics at room temperature. The measured dipole orientations align with the three-fold rotational symmetry of the h-BN lattice, and molecular dynamics in the liquid enivronment can be modulated electrochemically, suggesting a route for on-demand control of quantum emitters. We also find that lateral diffusion at the solid-liquid interface is far more dynamic than that of solid-state emitters. This simultaneous tracking of molecular conformation and photophysics advances the understanding of single-molecule interactions and enables real-time sensing through two-dimensional materials.

cond-mat.mes-hall↗

arXiv2024

Monitoring electrochemical dynamics through single-molecule imaging of hBN surface emitters in organic solvents

Electrochemical techniques conventionally lack spatial resolution and average local information over an entire electrode. While advancements in spatial resolution have been made through scanning probe methods, monitoring dynamics over large areas is still challenging, and it would be beneficial to be able to decouple the probe from the electrode itself. In this work, we leverage single molecule microscopy to spatiotemporally monitor analyte surface concentrations over a wide area using unmodified hexagonal boron nitride (hBN) in organic solvents. Through a sensing scheme based on redox-active species interactions with fluorescent emitters at the surface of hBN, we observe a linear decrease in the number of emitters under positive voltages applied to a nearby electrode. We find consistent trends in electrode reaction kinetics vs overpotentials between potentiostat-reported currents and optically-read emitter dynamics, showing Tafel slopes greater than 290 mV per decade. Finally, we draw on the capabilities of spectral single molecule localization microscopy (SMLM) to monitor the fluorescent species identity, enabling multiplexed readout. Overall, we show dynamic measurements of analyte concentration gradients at a micrometer-length scale with nanometer-scale depth and precision. Considering the many scalable options for engineering fluorescent emitters with 2D materials, our method holds promise for optically detecting a range of interacting species with unprecedented localization precision.

cond-mat.mes-hall↗

arXiv2024

CVD Graphene Contacts for Lateral Heterostructure MoS${_2}$ Field Effect Transistors

Intensive research is carried out on two-dimensional materials, in particular molybdenum disulfide, towards high-performance transistors for integrated circuits. Fabricating transistors with ohmic contacts is challenging due to the high Schottky barrier that severely limits the transistors' performance. Graphene-based heterostructures can be used in addition or as a substitute for unsuitable metals. We present lateral heterostructure transistors made of scalable chemical vapor-deposited molybdenum disulfide and chemical vapor-deposited graphene with low contact resistances of about 9 k$Ω$$μ$m and high on/off current ratios of 10${^8}$. We also present a theoretical model calibrated on our experiments showing further potential for scaling transistors and contact areas into the few nanometers range and the possibility of a strong performance enhancement by means of layer optimizations that would make transistors promising for use in future logic circuits.

cond-mat.mes-hall↗

arXiv2023

Nanofluidic logic with mechano-ionic memristive switches

While most neuromorphic systems are based on nanoscale electronic devices, nature relies on ions for energy-efficient information processing. Therefore, finding memristive nanofluidic devices is a milestone toward realizing electrolytic computers mimicking the brain down to its basic principles of operation. Here, we present a nanofluidic device designed for circuit scale in-memory processing that combines single-digit nanometric confinement and large entrance asymmetry. Our fabrication process is scalable while the device operates at the second timescale with a conductance ratio in the range 10-60. In-operando optical microscopy unveils the origin of memory, arising from the reversible formation of liquid blisters modulating the device conductance. The combination of features of these mechano-ionic memristive switches permits assembling logic circuits composed of two interactive devices and an ohmic resistor. These results open the way to design multi-component ionic machinery, such as nanofluidic neural networks, and implementing brain-inspired ionic computations.

cond-mat.soft↗

arXiv2023

Fluorescence Microscopy: a statistics-optics perspective

Fundamental properties of light unavoidably impose features on images collected using fluorescence microscopes. Modeling these features is ever more important in quantitatively interpreting microscopy images collected at scales on par or smaller than light's wavelength. Here we review the optics responsible for generating fluorescent images, fluorophore properties, microscopy modalities leveraging properties of both light and fluorophores, in addition to the necessarily probabilistic modeling tools imposed by the stochastic nature of light and measurement.

physics.optics↗

arXiv2023

Liquid-activated quantum emission from pristine hexagonal boron nitride for nanofluidic sensing

Liquids confined down to the atomic scale can show radically new properties. However, only indirect and ensemble measurements operate in such extreme confinement, calling for novel optical approaches enabling direct imaging at the molecular level. Here, we harness fluorescence originating from single-photon emitters at the surface of hexagonal boron nitride (hBN) for molecular imaging and sensing in nanometrically confined liquids. The emission originates from the chemisorption of organic solvent molecules onto native surface defects, revealing single-molecule dynamics at the interface through spatially correlated activation of neighboring defects. Emitter spectra further offer a direct readout of local dielectric properties, unveiling increasing dielectric order under nanometer-scale confinement. Liquid-activated native hBN defects bridge the gap between solid-state nanophotonics and nanofluidics, opening new avenues for nanoscale sensing and optofluidics.

cond-mat.mes-hall↗

arXiv2023

Large-Scale Integrated Vector-Matrix Multiplication Processor Based on Monolayer MoS2

Led by the rise of the internet of things, the world is experiencing exponential growth of generated data. Data-driven algorithms such as signal processing and artificial neural networks are required to process and extract meaningful information from it. They are, however, seriously limited by the traditional von-Neuman architecture with physical separation between processing and memory, motivating the development of in-memory computing. This emerging architecture is gaining attention by promising more energy-efficient computing on edge devices. In the past few years, two-dimensional materials have entered the field as a material platform suitable for realizing efficient memory elements for in-memory architectures. Here, we report a large-scale integrated 32x32 vector-matrix multiplier with 1024 floating-gate field-effect transistors (FGFET) that use monolayer MoS2 as the channel material. In our wafer-scale fabrication process, we achieve a high yield and low device-to-device variability, which are prerequisites for practical applications. A statistical analysis shows the potential for multilevel and analog storage with a single programming pulse, allowing our accelerator to be programmed using an efficient open-loop programming scheme. Next, we demonstrate reliable, discrete signal processing in a highly parallel manner. Our findings set the grounds for creating the next generation of in-memory processors and neural network accelerators that can take advantage of the full benefits of semiconducting van der Waals materials for non-von Neuman computing.

cond-mat.mes-hall↗

arXiv2022

Nanoscale thermal control of a single living cell enabled by diamond heater-thermometer

We report a new approach to controllable thermal stimulation of a single living cell and its compartments. The technique is based on the use of a single polycrystalline diamond particle containing silicon-vacancy (SiV) color centers. Due to the presence of amorphous carbon at its intercrystalline boundaries, such a particle is an efficient light absorber and becomes a local heat source when illuminated by a laser. Furthermore, the temperature of such a local heater is tracked by the spectral shift of the zero-phonon line of SiV centers [2]. Thus, the diamond particle acts simultaneously as a heater and a thermometer. In the current work, we demonstrate the ability of such a Diamond Heater-Thermometer (DHT) to locally alter the temperature, one of the numerous parameters that play a decisive role for the living organisms at the nanoscale. In particular, we show that the local heating of 11-12 °C relative to the ambient temperature (22 °C) next to individual HeLa cells and neurons, isolated from the mouse hippocampus, leads to a change in the intracellular distribution of the concentration of free calcium ions. For individual HeLa cells, a long-term (about 30 s) increase in the integral intensity of Fluo-4 NW fluorescence by about three times is observed, which characterizes an increase in the [Ca2+]cyt concentration of free calcium in the cytoplasm. Heating near mouse hippocampal neurons also caused a calcium surge - an increase in the intensity of Fluo-4 NW fluorescence by 30% and a duration of ~0.4 ms.

physics.bio-ph↗

arXiv2022

Elucidating contact electrification mechanism of water

The open water surface is known to be charged. Yet, the magnitude of the charge and the physical mechanism of the charging remain unclear, causing heated debates across the scientific community. Here we directly measure the charge Q of microdrops ejected from hydrophilic and hydrophobic capillaries and show that the water surface can take both positive or negative charge values depending on pH and the capillary type. Our experiments, theory, and simulations provide evidence that a junction of two aqueous interfaces with a different ion adsorption energy (e.g., liquid-solid and liquid-air interfaces) develops a pH-dependent contact potential difference {\Delta}{\phi} up to 52 mV. The longitudinal charge transfer between the interfaces stimulated by {\Delta}{\phi} determines the charge of the open water surface. The suggested static electrification mechanism provides far-reaching insights into the origin of electrical potentials in biological and electrochemical energy systems.

cond-mat.soft↗

arXiv2022

High-throughput nanopore fabrication and classification using FIB irradiation and automated pore edge analysis

Large-area nanopore drilling is a major bottleneck in state-of-the-art nanoporous 2D membrane fabrication protocols. In addition, high-quality structural and statistical descriptions of as-fabricated porous membranes are key to predicting the corresponding membrane-wide permeation properties. In this work, we investigate Xe-ion focused ion beam as a tool for scalable, large-area nanopore fabrication on atomically thin, free-standing molybdenum disulphide. The presented irradiation protocol enables designing ultrathin membranes with tunable porosity and pore dimension, along with spatial uniformity across large-area substrates. Fabricated nanoporous membranes were characterized using scanning transmission electron microscopy imaging and the observed nanopore geometries were analyzed through a pore-edge detection script. We further demonstrated that the obtained structural and statistical data can be readily passed on to computational and analytical tools to predict the permeation properties at both individual pore and membrane-wide scales. As an example, membranes featuring angstrom-scale pores were investigated in terms of their emerging water and ion flow properties through extensive all-atom molecular dynamics simulations. We believe that the combination of experimental and analytical approaches presented here should yield accurate physics-based property estimates and thus potentially enable a true function-by-design approach to fabrication for applications such as osmotic power generation, desalination/filtration, as well as their strain-tunable versions.

cond-mat.mtrl-sci↗

arXiv2022

Confinement-controlled Water Engenders High Energy Density Electrochemical-double-layer Capacitance

The renewable energy sector critically needs low-cost and environmentally neutral energy storage solutions throughout the entire device life cycle. However, the limited performance of standard water-based electrochemical systems prevents their use in specific applications. Meanwhile, recent fundamental studies revealed dielectric anomalies of water near solid-liquid interfaces of carbon-based nanomaterials. In contrast to the bulk water properties, these anomalies of water under nano-confinement and in the presence of electric fields have not yet been understood and used. Here, we experimentally study the ability of the interfacial water layer to engender and store charge in electrochemical double-layer capacitance. We demonstrate the prototype of a 'water only' membrane-electrode assembly. The prototype exhibits characteristics with a perspective of competing with existing batteries and supercapacitors without using electrolytes as ionic carriers. The results provide the impetus for developing high-energy-density electrochemical double-layer capacitors and open up other avenues for ecologically-neutral batteries, fuel cells, and nanofluidic devices.

physics.chem-ph↗

arXiv2021

Engineering optically active defects in hexagonal boron nitride using focused ion beam and water

Hexagonal boron nitride (hBN) has emerged as a promising material platform for nanophotonics and quantum sensing, hosting optically-active defects with exceptional properties such as high brightness and large spectral tuning. However, precise control over deterministic spatial positioning of emitters in hBN remained elusive for a long time, limiting their proper correlative characterization and applications in hybrid devices. Recently, focused ion beam (FIB) systems proved to be useful to engineer several types of spatially-defined emitters with various structural and photophysical properties. Here we systematically explore the physical processes leading to the creation of optically-active defects in hBN using FIB, and find that beam-substrate interaction plays a key role in the formation of defects. These findings are confirmed using transmission electron microscopy that reveals local mechanical deterioration of the hBN layers and local amorphization of ion beam irradiated hBN. Additionally, we show that upon exposure to water, amorphized hBN undergoes a structural and optical transition between two defect types with distinctive emission properties. Moreover, using super-resolution optical microscopy combined with atomic force microscopy, we pinpoint the exact location of emitters within the defect sites, confirming the role of defected edges as primary sources of fluorescent emission. This lays the foundation for FIB-assisted engineering of optically-active defects in hBN with high spatial and spectral control for applications ranging from integrated photonics, to quantum sensing to nanofluidics.

physics.optics↗