arXiv subjects

Alexander A. Khajetoorians

Publications and source records attributed to Alexander A. Khajetoorians.

At least 19 recordsLinked to original sources

arXiv2026

Collective excitation-mediated transport in nanoscale Josephson junctions that exhibit quantum confinement

Quantum confinement can strongly modify transport through Josephson junctions. Here, we study local tunneling transport through nanoscale Josephson junction stacks in the Coulomb blockade regime, where the metallic layers exhibit strong vertical quantum confinement. We find that quasiparticle transport is strongly enhanced by a collective excitation mode intrinsic to the junction and localized in the isolated metallic overlayer. We quantify both the collective-mode energy and the Coulomb gap and show that both exhibit strong layer-dependent modulation, consistent with the modulation of the underlying quantum well states. We further investigate how the collective excitation responds to various perturbations, including mechanical motion and an applied magnetic field. Our results suggest that this collective mode is sensitive to quasiparticles near the Fermi level and may therefore provide an indirect probe of the superconducting state.

cond-mat.supr-con↗

arXiv2026

Spin-orbit coupling by design in quantum state engineering of atomically defined quantum dots

Tuning spin-orbit coupling is essential in controlling both spin and charge in confined semiconductor nanostructures, yet it is rarely a truly controllable parameter. Here, we show control over the spin-orbit Hamiltonian in quantum dots and the resulting quantum states by tailoring the confinement potential with atomic-scale precision. Using scanning tunnelling microscopy and spectroscopy, we pattern individual Cs ions into designer quantum dot structures on the surface of indium antimonide, in which electrons from a two-dimensional electron gas are confined with chosen in-plane electric-field gradients. We then quantify the atomic level structure, both spatially resolving the orbital character of the electronic states and their magnetic-field evolution. We demonstrate that the level structure, including the induced zero-field splitting, can be tailored by the designed geometry of the local electric fields. These effects can be described using a Hamiltonian that allows consistent treatment of the confinement-induced spin-orbit coupling beyond the conventional Bychkov-Rashba description. This Hamiltonian is derived from a multiband k.p model and takes the energy dependence of the relevant physical parameters into account. Such precise control of spin-orbit coupling in semiconductor quantum dots is relevant to quantum and spintronic technologies.

cond-mat.mes-hall↗

arXiv2025

Influence of surface relaxations on scanning probe microscopy images of the charge density wave material 2H-NbSe$_2$

Scanning tunneling microscopy is the method of choice for characterizing charge density waves by imaging the variation in atomic-scale contrast of the surface. Due to the measurement principle of scanning tunneling microscopy, the electronic and lattice degrees of freedom are convoluted, making it difficult to disentangle a structural displacement from spatial variations in the electronic structure. In this work, we characterize the influence of the displacement of the surface-terminating Se atoms on the 3 x 3 charge density wave contrast in scanning probe microscopy images of 2H-NbSe$_2$. In scanning tunneling microscopy images, we observe the 3 x 3 charge density wave superstructure and atomic lattice at all probed tip-sample distances. In contrast, non-contact atomic force microscopy images show both periodicities only at small tip-sample distances while, unexpectedly, a 3 x 3 superstructure is present at larger tip-sample distances. Using density functional theory calculations, we qualitatively reproduce the experimental findings and indicate that the 3 x 3 superstructure at different tip-sample distances in non-contact atomic force microscopy images is a result from different underlying interactions. In addition, we show that the displacement of the surface-terminating Se atoms has a negligible influence to the contrast in scanning tunneling microscopy images. Our combined experimental and theoretic work presents a method on how to discriminate the influence of the surface corrugation from the variation of the charge density to the charge density wave contrast in scanning probe microscopy images, which can provide insights into the influence of structural disorder to a charge density wave ground state.

cond-mat.mes-hall↗

arXiv2024

Activating the fluorescence of a Ni(II) complex by energy transfer

Luminescence of open-shell 3d metal complexes is often quenched due to ultrafast intersystem crossing (ISC) and cooling into a dark metal-centered excited state. We demonstrate successful activation of fluorescence from individual nickel phthalocyanine (NiPc) molecules in the junction of a scanning tunneling microscope (STM) by resonant energy transfer from other metal phthalocyanines at low temperature. By combining STM, scanning tunneling spectroscopy, STM- induced luminescence, and photoluminescence experiments as well as time-dependent density functional theory, we provide evidence that there is an activation barrier for the ISC, which in most experimental conditions is overcome. We show that this is also the case in an electroluminescent tunnel junction where individual NiPc molecules adsorbed on an ultrathin NaCl decoupling film on a Ag(111) substrate are probed. However, when placing an MPc (M = Zn, Pd, Pt) molecule close to NiPc by means of STM atomic manipulation, resonant energy transfer can excite NiPc without overcoming the ISC activation barrier, leading to Q-band fluorescence. This work demonstrates that the thermally activated population of dark metal-centered states can be avoided by a designed local environment at low temperatures paired with a directed molecular excitation into vibrationally cold electronic states. Thus, we can envisage the use of luminophores based on more abundant transition metal complexes that do not rely on Pt or Ir.

cond-mat.mes-hall↗

arXiv2023

Bipolar single-molecule electroluminescence and electrofluorochromism

Understanding the fundamental mechanisms of optoelectronic excitation and relaxation pathways on the single-molecule level has only recently been started by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced luminescence (STML). In this paper, we investigate cationic and anionic fluorescence of individual zinc phthalocyanine (ZnPc) molecules adsorbed on ultrathin NaCl films on Ag(111) by using STML. They depend on the tip-sample bias polarity and appear at threshold voltages that are correlated with the onset energies of particular molecular orbitals, as identified by STS. We also find that the fluorescence is caused by a single electron tunneling process. Comparing with results from density functional theory calculations, we propose an alternative many-body picture to describe the charging and electroluminescence mechanism. Our study provides aspects toward well-defined voltage selectivity of bipolar electrofluorochromism, as well as fundamental insights regarding the role of transiently charged states of emitter molecules within OLED devices.

cond-mat.mes-hall↗

arXiv2022

Orbital memory from individual Fe atoms on black phosphorus

Bistable valency in individual atoms presents a new approach toward single-atom memory, as well as a building block to create tunable and stochastic multi-well energy landscapes. Yet, this concept of orbital memory has thus far only been observed for cobalt atoms on the surface of black phosphorus, which are switched using tip-induced ionization. Here, we show that individual iron atoms on the surface of black phosphorus exhibit orbital memory using a combination of scanning tunneling microscopy and spectroscopy with ab initio calculations based on density functional theory. Unlike cobalt, the iron orbital memory can be switched in its non-ionized ground state. Based on calculations, we confirm that each iron valency has a distinct magnetic moment that is characterized by a distinguishable charge distribution due to the different orbital population. By studying the stochastic switching of the valency with varying tunneling conditions, we propose that the switching mechanism is based on a two-electron tunneling process.

cond-mat.mes-hall↗

arXiv2022

Gating orbital memory with an atomic donor

Orbital memory is defined by two stable valencies that can be electrically switched and read-out. To explore the influence of an electric field on orbital memory, we studied the distance-dependent influence of an atomic Cu donor on the state favorability of an individual Co atom on black phosphorus. Using low temperature scanning tunneling microscopy/spectroscopy, we characterized the electronic properties of individual Cu donors, corroborating this behavior with ab initio calculations based on density functional theory. We studied the influence of an individual donor on the charging energy and stochastic behavior of an individual Co atom. We found a strong impact on the state favorability in the stochastic limit. These findings provide quantitative information about the influence of local electric fields on atomic orbital memory.

cond-mat.mes-hall↗

arXiv2021

An atomic Boltzmann machine capable of on-chip learning

The Boltzmann Machine (BM) is a neural network composed of stochastically firing neurons that can learn complex probability distributions by adapting the synaptic interactions between the neurons. BMs represent a very generic class of stochastic neural networks that can be used for data clustering, generative modelling and deep learning. A key drawback of software-based stochastic neural networks is the required Monte Carlo sampling, which scales intractably with the number of neurons. Here, we realize a physical implementation of a BM directly in the stochastic spin dynamics of a gated ensemble of coupled cobalt atoms on the surface of semiconducting black phosphorus. Implementing the concept of orbital memory utilizing scanning tunnelling microscopy, we demonstrate the bottom-up construction of atomic ensembles whose stochastic current noise is defined by a reconfigurable multi-well energy landscape. Exploiting the anisotropic behaviour of black phosphorus, we build ensembles of atoms with two well-separated intrinsic time scales that represent neurons and synapses. By characterizing the conditional steady-state distribution of the neurons for given synaptic configurations, we illustrate that an ensemble can represent many distinct probability distributions. By probing the intrinsic synaptic dynamics, we reveal an autonomous reorganization of the synapses in response to external electrical stimuli. This self-adaptive architecture paves the way for on-chip learning directly in atomic-scale machine learning hardware.

cond-mat.mes-hall↗

arXiv2021

Thermally-induced magnetic order from glassiness in elemental neodymium

Temperature in thermodynamics is synonymous with disorder, and responsible for ultimately destroying ordered phases. Here, we show an unusual magnetic transition where, with increasing the temperature of elemental neodymium, long-range multi-Q magnetic order emerges from a self-induced spin glass. Using temperature-dependent spin-polarized scanning tunneling microscopy, we characterize the local Q order in the spin-Q glass phase and quantify the emergence of long-range multi-Q order with increasing temperature. We develop two distinct analysis tools, which enable the quantification of the glass transition temperature, based on measured spatially-dependent magnetization. We compare these observations with atomic spin dynamics simulations, which reproduce the qualitative observation of a phase transition from a low-temperature spin glass phase to an intermediate ordered multi-Q phase. These simulations trace the origin of the unexpected high temperature order in weakened frustration driven by temperature-dependent sublattice correlations. These findings constitute an example of order from disorder and provide a rich platform to study magnetization dynamics in a self-induced spin glass.

cond-mat.mtrl-sci↗

arXiv2021

Quantifying the interplay between fine structure and geometry of an individual molecule on a surface

The pathway toward the tailored synthesis of materials starts with precise characterization of the conformational properties and dynamics of individual molecules. Electron spin resonance based scanning tunneling microscopy can potentially address molecular structure with unprecedented resolution. Here, we determine the fine structure and geometry of an individual TiH molecule, utilizing a combination of a newly developed mK ESR-STM in a vector magnetic field and ab initio approaches. We demonstrate a strikingly large anisotropy of the g-tensor unusual for a spin doublet ground state, resulting from a non-trivial orbital angular momentum stemming from the molecular ground state. We quantify the relationship between the resultant fine structure, hindered rotational modes, and orbital excitations. Our model system provides new avenues to determine the structure and dynamics of individual molecules.

cond-mat.mes-hall↗

arXiv2021

Moiré induced electronic structure modifications in monolayer V$_{2}$S$_{3}$ on Au(111)

There is immense interest in how the local environment influences the electronic structure of materials at the single layer limit. We characterize moiré induced spatial variations in the electronic structure of in-situ grown monolayer V2S3 on Au(111) by means of low temperature scanning tunneling microscopy and spectroscopy. We observe a long-range modulation of the integrated local density of states (LDOS), and quantify this modulation with respect to the moiré superstructure for multiple orientations of the monolayer with respect to the substrate. Scanning tunneling spectroscopy reveals a prominent peak in the LDOS, which is shifted in energy at different points of the moiré superstructure. Comparing ab initio calculations with angle-resolved photoemission, we are able to attribute this peak to bands that exhibit a large out-of-plane d-orbital character. This suggests that the moiré driven variations in the measured density of states is driven by a periodic modulation of the monolayer-substrate hybridization.

cond-mat.mtrl-sci↗

arXiv2020

A scanning tunneling microscope capable of electron spin resonance and pump-probe spectroscopy at mK temperature and in vector magnetic field

In the last decade, detecting spin dynamics at the atomic scale has been enabled by combining techniques like electron spin resonance (ESR) or pump-probe spectroscopy with scanning tunneling microscopy (STM). Here, we demonstrate an ultra-high vacuum (UHV) STM operational at milliKelvin (mK) and in a vector magnetic field capable of both ESR and pump-probe spectroscopy. By implementing GHz compatible cabling, we achieve appreciable RF amplitudes at the junction while maintaining mK base temperature. We demonstrate the successful operation of our setup by utilizing two experimental ESR modes (frequency sweep and magnetic field sweep) on an individual TiH molecule on MgO/Ag(100) and extract the effective g-factor. We trace the ESR transitions down to MHz into an unprecedented low frequency band enabled by the mK base temperature. We also implement an all-electrical pump-probe scheme based on waveform sequencing suited for studying dynamics down to the nanoseconds range. We benchmark our system by detecting the spin relaxation time T1 of individual Fe atoms on MgO/Ag(100) and note a field strength and orientation dependent relaxation time.

cond-mat.mes-hall↗

arXiv2020

Plasmon-driven motion of an individual molecule

We demonstrate that nanocavity plasmons generated a few nanometers away from a molecule can induce molecular motion. For this, we study the well-known rapid shuttling motion of zinc phthalocyanine molecules adsorbed on ultrathin NaCl films by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced light emission. Comparing spatially resolved single-molecule luminescence spectra from molecules anchored to a step edge with isolated molecules adsorbed on the free surface, we found that the azimuthal modulation of the Lamb shift is diminished in case of the latter. This is evidence that the rapid shuttling motion is remotely induced by plasmon-exciton coupling. Plasmon-induced molecular motion may open an interesting playground to bridge the nanoscopic and mesoscopic worlds by combining molecular machines with nanoplasmonics to control directed motion of single molecules without the need for local probes.

cond-mat.mes-hall↗

arXiv2020

Self-induced spin glass state in elemental and crystalline neodymium

Spin glasses are a highly complex magnetic state of matter, intricately linked to spin frustration and structural disorder. They exhibit no long-range order and exude aging phenomena, distinguishing them from quantum spin liquids. We report a new type of spin glass state, the spin-Q glass, observable in bulk-like crystalline metallic neodymium thick films. Using spin-polarized scanning tunneling microscopy combined with ab initio calculations and atomistic spin-dynamics simulations, we visualize the variations in atomic-scale non-collinear order and its response to magnetic field and temperature. We quantify the aging phenomena relating the glassiness to crystalline symmetry and the energy landscape. This result not only resolves the long-standing debate of the magnetism of neodymium, but also suggests that glassiness may arise in other magnetic solids lacking extrinsic disorder.

cond-mat.mtrl-sci↗

arXiv2020

Quantifying Exchange Forces of a Non-Collinear Magnetic Structure on the Atomic Scale

The large interest in chiral magnetic structures for realization of nanoscale magnetic storage or logic devices has necessitated methods which can quantify magnetic interactions at the atomic scale. To overcome the limitations of the typically used current-based sensing of atomic-scale exchange interactions, a force-based detection scheme is highly advantageous. Here, we quantify the atomic-scale exchange force field between a ferromagnetic tip and a cycloidal spin spiral using our developed combination of current and exchange force detection. Compared to the surprisingly weak spin polarization, the exchange force field is more sensitive to atomic-scale variations in the magnetization. First-principles calculations reveal that the measured atomic-scale variations in the exchange force originate from different contributions of direct and indirect (Zener) type exchange mechanisms, depending on the chemical tip termination. Our work opens the perspective of quantifying different exchange mechanisms of chiral magnetic structures with atomic-scale precision using 3D magnetic exchange force field measurements.

cond-mat.mes-hall↗

arXiv2019

Atom-by-atom construction of attractors in a tunable finite size spin array

We demonstrate that a two-dimensional finite and periodic array of Ising spins coupled via RKKY-like exchange can exhibit tunable magnetic states ranging from three distinct magnetic regimes: (1) a conventional ferromagnetic regime, (2) a glass-like regime, and (3) a new multi-well regime. These magnetic regimes can be tuned by one gate-like parameter, namely the ratio between the lattice constant and the oscillating interaction wavelength. We characterize the various magnetic regimes, quantifying the distribution of low energy states, aging relaxation dynamics, and scaling behavior. The glassy and multi-well behavior results from the competing character of the oscillating long-range exchange interactions. The multi-well structure features multiple attractors, each with a sizable basin of attraction. This may open the possible application of such atomic arrays as associative memories.

cond-mat.stat-mech↗

arXiv2019

Anisotropic two-dimensional screening at the surface of black phosphorus

Screening in reduced dimensions has strong consequences on the electronic properties in van der Waals semiconductors, impacting the quasiparticle band gap and exciton binding energy. Screening in these materials is typically treated isotropically, yet black phosphorus exhibits in-plane electronic anisotropy seen in its effective mass, carrier mobility, excitonic wavefunctions, and plasmonic dispersion. Here, we use the adsorption of individual potassium atoms on the surface of black phosphorus to vary the near-surface doping over a wide range, while simultaneously probing the dielectric screening via the ordering of the adsorbed atoms. Using scanning tunneling microscopy, we visualize the role of strongly anisotropic screening which leads to the formation of potassium chains with a well-defined orientation and spacing. We quantify the mean interaction potential utilizing statistical methods and find that the dimensionality and anisotropy of the screening is consistent with the presence of a band-bending induced confinement potential near the surface. We corroborate the observed behavior with coverage-dependent studies of the electronic structure with angle-resolved photoemission.

cond-mat.mes-hall↗

arXiv2019

Designer quantum states of matter created atom-by-atom

With the advances in high resolution and spin-resolved scanning tunneling microscopy as well as atomic-scale manipulation, it has become possible to create and characterize quantum states of matter bottom-up, atom-by-atom. This is largely based on controlling the particle- or wave-like nature of electrons, as well as the interactions between spins, electrons, and orbitals and their interplay with structure and dimensionality. We review the recent advances in creating artificial electronic and spin lattices that lead to various exotic quantum phases of matter, ranging from topological Dirac dispersion to complex magnetic order. We also project future perspectives in non-equilibrium dynamics, prototype technologies, engineered quantum phase transitions and topology, as well as the evolution of complexity from simplicity in this newly developing field.

cond-mat.mes-hall↗