arXiv subjects

Pavel Jelínek

Publications and source records attributed to Pavel Jelínek.

At least 19 recordsLinked to original sources

arXiv2026

Atomic-scale control of substrate-spin coupling via vertical manipulation of a 2D metal-organic framework

Two-dimensional (2D) materials with frustrated crystal geometries can host strongly correlated electrons, potentially leading to a range of exotic many-body quantum phases such as Mott insulators, quantum spin-liquids, and Kondo lattices. The ability to control exchange-coupling within these systems is therefore highly desirable. Here, we use an atomically sharp scanning tunneling microscope probe to vertically manipulate a 2D Mott insulating kagome metal-organic framework (MOF) featuring Kondo-screened local magnetic moments on Ag(111). We show that by controlling the adsorption height of the MOF, we can also controllably and reversibly change the strength of Kondo coupling between the MOF's local spins and the substrate's conduction electrons. This mechanical control of Kondo coupling could be extended to other forms of interlayer exchange coupling, potentially allowing for atomic-scale design or control of spintronics technologies.

cond-mat.str-el↗

arXiv2026

Topological Engineering of a Frustrated Antiferromagnetic Triradical in Aza-Triangulene Architectures

Open-shell nanographenes provide a versatile platform to host unconventional magnetic states within their π-conjugated networks. Particularly appealing are graphene architectures that incorporate spatially separated radicals and tunable interactions, offering a scalable route toward spin-based quantum architectures. Triangulenes are ideal for this purpose, as their radical count scales with size, although strong hybridization prevents individual spin control. Here, we realize a radical reconfiguration strategy that transforms a single-radical aza-triangulene into three topologically protected spin states by covalently extending it with armchair anthene moieties of increasing length. Scanning tunnelling spectroscopy reveals emergent correlated spins forming a frustrated spin trimer whose interaction weakens with anthene length. This trend is captured by multi-reference electronic-structure calculations, which trace a progressive rise in polyradical character driven by the progressive reorganization of the correlated frontier orbitals into three edge-localized natural orbitals. Consequently, the initial single-radical doublet reorganizes into non-interacting edge spins, a molecular analog of a three-qubit quantum register.

cond-mat.mes-hall↗

arXiv2025

Breaking Peierls theorem in polyacetylene chains via topological design

Peierls theorem postulates that a one-dimensional (1D) metallic chain must undergo a metal-to-insulator transition via lattice distortion, resulting in bond length alternation (BLA) within the chain. The validity of this theorem has been repeatedly proven in practice, as evidenced by the absence of a metallic phase in low-dimensional atomic lattices and electronic crystals, including conjugated polymers, artificial 1D quantum nanowires, and anisotropic inorganic crystals. Overcoming this transition enables realizing long-sought organic quantum phases of matter, including 1D synthetic organic metals and even high-temperature organic superconductors. Herein, we demonstrate that the Peierls transition can be globally suppressed by employing lattice topology engineering of classic trans-polyacetylene chains connected to open-shell nanographene terminals. The appropriate topology connection enables an effective interplay between the zero-energy modes (ZMs) of terminal and the finite odd-membered polyacetylene (OPA) chains. This creates a critical topology-defined highest occupied molecular orbital (HOMO) that compensates for bond density variations, thereby suppressing BLA and reestablishing their quasi-1D metallic character. Moreover, it also causes the formation of an unconventional boundary-free resonance state, being delocalized over the entire chain with non-decaying spectral weight, distinguishing them from traditional solitons observed in polyacetylene. Our finding sets the stage for pioneering the suppression of material instability and the creation of synthetic organic quantum materials with unconventional quantum phases previously prohibited by the Peierls transition.

cond-mat.mes-hall↗

arXiv2025

On-surface Synthesis of a Ferromagnetic Molecular Spin Trimer

Triangulenes are prototypical examples of open-shell nanographenes. Their magnetic properties, arising from the presence of unpaired $π$ electrons, can be extensively tuned by modifying their size and shape or by introducing heteroatoms. Different triangulene derivatives have been designed and synthesized in recent years, thanks to the development of on-surface synthesis strategies. Triangulene-based nanostructures with polyradical character, hosting several interacting spin units, can be challenging to fabricate but are particularly interesting for potential applications in carbon-based spintronics. Here, we combine pristine and N-doped triangulenes into a more complex nanographene, \textbf{TTAT}, predicted to possess three unpaired $π$ electrons delocalized along the zigzag periphery. We generate the molecule on an Au(111) surface and detect direct fingerprints of multi-radical coupling and high-spin state using scanning tunneling microscopy and spectroscopy. With the support of theoretical calculations, we show that its three radical units are localized at distinct parts of the molecule and couple via symmetric ferromagnetic interactions, which result in a $S=3/2$ ground state, thus demonstrating the realization of a molecular ferromagnetic Heisenberg-like spin trimer

cond-mat.mes-hall↗

arXiv2025

Magnetic ground state discrimination of a Polyradical Nanog-raphene using Nickelocene-Functionalized Tips

Molecular magnets are a promising class of materials with exciting properties and applications. However, a profound understanding and application of such materials depends on the accurate detection of their electronic and magnetic properties. Despite the availability of experimental techniques that can sense the magnetic signal, the exact determination of the spin ground states and spatial distribution of exchange interaction of strongly correlated single-molecule magnets remains challenging. Here, we demonstrate that scanning probe microscopy with a nickelocene-functionalized probe can distinguish between nearly degenerate multireference ground states of single-molecule π-magnets and map their spatial distribution of the exchange interaction. This method expands the already outstanding imaging capabilities of scanning probe microscopy for characterizing the chemical and electronic structures of individual molecules, paving the way for the study of strongly correlated molecular magnets with unprecedented spatial resolution.

cond-mat.mtrl-sci↗

arXiv2024

Theoretical model for multi-orbital Kondo screening in strongly correlated molecules with several unpaired electrons

The mechanism of Kondo screening in strongly correlated molecules with several unpaired electrons on a metal surface is still under debate. Here, we provide a theoretical framework that rationalizes the emergence of Kondo screening involving several extended molecular orbitals with unpaired electrons. We introduce a perturbative model, which provides simple rules to identify the presence of antiferromagnetic spin-flip channels involving charged molecular multiplets responsible for Kondo screening. The Kondo regime is confirmed by numerical renormalization group calculations. In addition, we introduce the concept of Kondo orbitals as molecular orbitals associated with the Kondo screening process, which provide a direct interpretation of experimental $dI/dV$ maps of Kondo resonances. We demonstrate that this theoretical framework can be applied to different strongly correlated open-shell molecules on metal surfaces, obtaining good agreement with previously published experimental data.

cond-mat.str-el↗

arXiv2024

Photocleavage of aliphatic C--C bonds in the interstellar medium

Ultraviolet (UV) processing in the insterstellar medium (ISM) induces the dehydrogenation of hydrocarbons. Aliphatics, including alkanes, are present in different interstellar environments, being prevalently formed in evolved stars; thus, the dehydrogenation by UV photoprocessing of alkanes plays an important role in the chemistry of the ISM, leading to the formation of unsaturated hydrocarbons and eventually to aromatics, the latter ubiquitously detected in the ISM. Here, through combined experimental results and \textit{ab-initio} calculations, we show that UV absorption (mainly at the Ly-$α$ emission line of hydrogen at 121.6 nm) promotes an alkane to an excited Rydberg state from where it evolves towards fragmentation inducing the formation of olefinic C=C bonds, which are necessary precursors of aromatic hydrocarbons. We show that photochemistry of aliphatics in the ISM does not primarily produce direct hydrogen elimination but preferential C-C photocleavage. Our results provide an efficient synthetic route for the formation of unsaturated aliphatics, including propene and dienes, and suggest that aromatics could be formed in dark clouds by a bottom-up mechanism involving molecular fragments produced by UV photoprocessing of aliphatics.

astro-ph.GA↗

arXiv2024

Unveiling the inter-layer interaction in a 1H/1T TaS$_2$ van de Waals heterostructure

This study delves into the intriguing properties of 1H/1T-TaS$_2$ van der Waals heterostructure, focusing on the transparency of the 1H layer to the Charge Density Wave of the underlying 1T layer. Despite the sizable interlayer separation and metallic nature of the 1H layer, positive bias voltages result in a pronounced superposition of the 1T charge density wave structure on the 1H layer. The conventional explanation relying on tunneling effects proves insufficient. Through a comprehensive investigation combining lowtemperature scanning tunneling microscopy, scanning tunneling spectroscopy, non-contact atomic force microscopy, and firstprinciples calculations, we propose an alternative interpretation. The transparency effect arises from a weak yet substantial electronic coupling between the 1H and 1T layers, challenging prior understanding of the system. Our results highlight the critical role played by interlayer electronic interactions in van der Waals heterostructures to determine the final ground states of the systems.

cond-mat.str-el↗

arXiv2023

Multi-orbital Kondo screening in strongly correlated polyradical nanographenes

We discuss coexistence of Kondo and spin excitation signals in tunneling spectroscopy in strongly correlated polyradical $π$-magnetic nanographenes on a metal surface. The Kondo signal is rationalized by a multi-orbital Kondo screening of the unpaired electrons. The fundamental processes are spin-flips of antiferromagnetic (AFM) order involving charged molecular multiplets. We introduce a~perturbative model, which provides simple rules to identify the presence of AFM channels responsible for Kondo screening. The Kondo regime is confirmed by numerical renormalization group calculations. This framework can be applied to similar strongly correlated open-shell systems.

cond-mat.str-el↗

arXiv2023

Chemisorption Induced Formation of Biphenylene Dimer on Surfaces

We report an example that demonstrates the clear interdependence between surface-supported reactions and molecular adsorption configurations. Two biphenyl-based molecules with two and four bromine substituents, i.e. 2,2-dibromo-biphenyl (DBBP) and 2,2,6,6-tetrabromo-1,1-biphenyl (TBBP), show completely different reaction pathways on a Ag(111) surface, leading to the selective formation of dibenzo[e,l]pyrene and biphenylene dimer, respectively. By combining low-temperature scanning tunneling microscopy, synchrotron radiation photoemission spectroscopy, and density functional theory calculations, we unravel the underlying reaction mechanism. After debromination, a bi-radical biphenyl can be stabilized by surface Ag adatoms, while a four-radical biphenyl undergoes spontaneous intramolecular annulation due to its extreme instability on Ag(111). Such different chemisorption-induced precursor states between DBBP and TBBP consequently lead to different reaction pathways after further annealing. In addition, using bond-resolving scanning tunneling microscopy and scanning tunneling spectroscopy, we determine the bond length alternation of biphenylene dimer product with atomic precision, which contains four-, six-, and eight-membered rings. The four-membered ring units turn out to be radialene structures.

cond-mat.mtrl-sci↗

arXiv2022

The Role of the Magnetic Anisotropy in Atomic-Spin Sensing of 1D Molecular Chains

One-dimensional metal-organic chains often possess a complex magnetic structure susceptible to be modified by a alteration of their chemical composition. The possibility to tune their magnetic properties provides an interesting playground to explore quasiparticle interactions in low-dimensional systems. Despite the great effort invested so far, a detailed understanding of the interactions governing the electronic and magnetic properties of the low-dimensional systems is still incomplete. One of the reasons is the limited ability to characterize their magnetic properties at the atomic scale. Here, we provide a comprehensive study of the magnetic properties of metal-organic one-dimensional (1D) coordination polymers consisting of 2,5-diamino-1,4-benzoquinonediimine ligands coordinated with Co or Cr atoms synthesized in ultra-high vacuum conditions on a Au(111) surface. A combination of an integral X-ray spectroscopy with local-probe inelastic electron tunneling spectroscopy corroborated by multiplet analysis, density functional theory, and inelastic electron tunneling simulations enable us to obtain essential information about their magnetic structure, including the spin magnitude and orientation at the magnetic atoms, as well as the magnetic anisotropy.

cond-mat.mes-hall↗

arXiv2021

Sub-angstrom Non-invasive Imaging of Atomic Arrangement in 2D Hybrid Perovskites

Non-invasive imaging of the atomic arrangement in two-dimensional (2D) Ruddlesden-Popper hybrid Perovskites (RPPs), as well as understanding the related effects is challenging, due to the insulating nature and softness of the organic layers which also obscure the underlying inorganic lattice. Here, we demonstrate a sub-angstrom resolution imaging of both soft organic layers and inorganic framework in a prototypical 2D lead-halide RPP crystal via combined tip-functionalized Scanning Tunneling Microscopy (STM) and non-contact Atomic Force Microscope (ncAFM) corroborated by theoretical simulations. STM measurements unveil the atomic reconstruction of the inorganic lead-halide lattice and overall twin-domain composition of the RPP crystal, while ncAFM measurements with a CO-tip enable non-perturbative visualization of the cooperative reordering of surface organic cations driven by their hydrogen bonding interactions with the inorganic lattice. Moreover, such a joint technique also allows for the atomic-scale imaging of the electrostatic potential variation across the twin-domain walls, revealing alternating quasi-one-dimensional (1D) electron and hole-channels at neighboring twin-boundaries, which may influence in-plane exciton transport and dissociation.

cond-mat.mtrl-sci↗

arXiv2021

Resolving Ambiguity of the Kondo Temperature Determination in Mechanically Tunable Single-Molecule Kondo Systems

Determination of the molecular Kondo temperature $T_K$ poses a challenge in most cases when the experimental temperature cannot be tuned to a sufficient extent. We show how this ambiguity can be resolved if additional control parameters are present, such as magnetic field and mechanical gating. We record the evolution of the differential conductance by lifting an individual molecule from the metal surface with the tip of a scanning tunneling microscope. By fitting the measured conductance spectra with the single impurity Anderson model we are able to demonstrate that the lifting tunes the junction continuously from the strongly correlated Kondo-singlet to the free spin $1/2$ ground state. In the crossover regime, where $T_K$ is similar to the temperature of experiment, the fitting yields ambiguous estimates of $T_K$ varying by an order of magnitude. We show that analysis of the conductance measured in two distinct external magnetic fields can be used to resolve this problem.

cond-mat.mes-hall↗

arXiv2021

Electronic Self-passivation of Single Vacancy in Black Phosphorus via a Controlled Ionization

We report that mono-elemental black phosphorus presents a new electronic self-passivation scheme of single vacancy (SV). By means of low-temperature scanning tunneling microscopy and bond-resolved non-contact atomic force microscopy, we demonstrate that the local reconstruction and ionization of SV into negatively charged $\mathrm{SV}^-$ leads to the passivation of dangling bonds and thus the quenching of in-gap states, which can be achieved by mild thermal annealing or STM tip manipulation. SV exhibits a strong and symmetric Friedel oscillation (FO) pattern, while $\mathrm{SV}^-$ shows an asymmetric FO pattern with local perturbation amplitude reduced by one order of magnitude and a faster decay rate. The enhanced passivation by forming $\mathrm{SV}^-$ can be attributed to its weak dipole-like perturbation, consistent with density-functional theory and numerical calculations. Therefore, self-passivated $\mathrm{SV}^-$ is electronically benign and acts as a much weaker scattering center, which may hold the key to further enhance the charge mobility of BP and its analogs.

cond-mat.mtrl-sci↗

arXiv2020

Significance of nuclear quantum effects in hydrogen bonded molecular chains

In hydrogen bonded systems, nuclear quantum effects such as zero-point motion and tunneling can significantly affect their material properties through underlying physical and chemical processes. Presently, direct observation of the influence of nuclear quantum effects on the strength of hydrogen bonds with resulting structural and electronic implications remains elusive, leaving opportunities for deeper understanding to harness their fascinating properties. We studied hydrogen-bonded one-dimensional quinonediimine molecular networks which may adopt two isomeric electronic configurations via proton transfer. Herein, we demonstrate that concerted proton transfer promotes a delocalization of π-electrons along the molecular chain, which enhances the cohesive energy between molecular units, increasing the mechanical stability of the chain and giving rise to new electronic in-gap states localized at the ends. These findings demonstrate the identification of a new class of isomeric hydrogen bonded molecular systems where nuclear quantum effects play a dominant role in establishing their chemical and physical properties. We anticipate that this work will open new research directions towards the control of mechanical and electronic properties of low-dimensional molecular materials via concerted proton tunneling.

cond-mat.mes-hall↗

arXiv2020

Steering alkyne homocoupling with on-surface synthesized catalysts

We report a multi-step on-surface synthesis strategy. The first step consists in the surface-supported synthesis of metal-organic complexes, which are subsequently used as catalysts to steer on-surface alkyne coupling reactions. In addition, we analyze and compare the electronic properties of the different coupling motifs obtained.

cond-mat.mtrl-sci↗

arXiv2020

Tailoring π-conjugation and vibrational modes to steer on-surface synthesis of pentalene-bridged ladder polymers

The development of synthetic strategies to engineer π-conjugated polymers is of paramount importance in modern chemistry and materials science. Here we introduce a theoretical and experimental synthetic paradigm based on the search for specific vibrational modes through an appropriate tailoring of the π-conjugation of the precursors, in order to increase the attempt frequency of a chemical reaction. First, we on-surface design a 1D π-conjugated polymer with specific π-topology, which is based on bisanthene monomers linked by cumulene bridges that tune specific vibrational modes. In a second step, upon further annealing, such vibrational modes steer the two-fold cyclization reaction between adjacent bisanthene moieties, which gives rise to a long and free-defect pentalene-bridged conjugated ladder polymer featuring a low band gap. In addition, high resolution atomic force microscopy allows us to identify by atomistic insights the resonant form of the polymer, thus confirming the validity of the Glidewell and Lloyd's rules for aromaticity. This on-surface synthetic strategy may stimulate exploiting previously precluded reactions towards novel pi-conjugated polymers with specific structures and properties.

cond-mat.mes-hall↗

arXiv2018

Identification of two-dimensional $FeO_2$ termination of hematite $α-Fe_2O_3(0001)$ surface

Iron oxides are among the most abundant compounds on Earth and have consequently been studied and used extensively in industrial processes. Despite these efforts, concrete understanding of some of their surface phase structures has remained elusive, in particular the oxidized $α-Fe_2O_3(0001)$ hematite surface. We detail an optimized recipe to produce this phase over the entire hematite surface and study the geometrical parameters and composition of its complex structure by means of atomically resolved microscopy, electron diffraction and surface-sensitive spectroscopies. We conclude that the oxidized $α-Fe_2O_3(0001)$ surface is terminated by a two-dimensional iron oxide with structure, lattice parameters, and orientation different from the bulk substrate. Using total-energy density functional theory for simulation of a large-scale atomic model, we identify the structure of the surface layer as antiferromagnetic, conductive $1T-FeO_2$ attached on half-metal terminated bulk. The model succeeds in reproducing the characteristic modulations observed in the atomically resolved images and electron diffraction patterns.

cond-mat.mtrl-sci↗