Atomistic simulation of the FEBID-driven growth of iron-based nanostructures

Prosvetov, Alexey; Verkhovtsev, Alexey V.; Sushko, Gennady B.; Solov’yov, Andrey V.

doi:10.1039/d2cp00809b

Cited by 4 publications

(21 citation statements)

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“…The process of quenching is similar to that observed here by the argon cluster. Understanding irradiation-driven fragmentation patterns for molecular systems in environments facilitates the advancement of advanced computational models for studying irradiation-induced chemistry processes involving complex molecular systems. ,,, …”

Section: Discussionmentioning

confidence: 99%

“…Electron-induced decomposition of adsorbed precursor molecules releases organic ligands, resulting in the clusterization of the precursor’s metallic component on a surface. The fundamental physicochemical phenomena that govern the formation, growth, and composition of deposits grown by FEBID still need to be fully understood and are the subject of ongoing research. − Achieving this goal requires a concerted approach linking fundamental knowledge of electron-driven chemistry in FEBID with rational design and synthesis of novel precursor molecules …”

Section: Introductionmentioning

confidence: 99%

“…These computational methodologies enable to embed random, fast, and local quantum transformations occurring in molecular systems due to chemical reactions or irradiation-induced quantum processes (e.g., bond breakage via DI or DEA) into the classical MD framework. This provides possibilities for simulations of chemical and irradiation-driven transformations of various molecular, biomolecular, and nano systems on the temporal and spatial scales inaccessible for simulations based on the ab initio quantum methods. ,,,− Major dissociative transformations of irradiated molecular systems (such as molecular topology changes, redistribution of atomic partial charges, or alteration of interatomic interactions) are simulated by means of MD with reactive force fields, particularly the reactive CHARMM (rCHARMM) force field implemented in MBN Explorer.…”

Section: Introductionmentioning

confidence: 99%

“…The fundamental physicochemical phenomena that govern the formation, growth, and composition of deposits grown by FEBID still need to be fully understood and are the subject of ongoing research. 14 − 16 Achieving this goal requires a concerted approach linking fundamental knowledge of electron-driven chemistry in FEBID 17 with rational design and synthesis of novel precursor molecules. 18 …”

Section: Introductionmentioning

confidence: 99%

“…This provides possibilities for simulations of chemical and irradiation-driven transformations of various molecular, biomolecular, and nano systems on the temporal and spatial scales inaccessible for simulations based on the ab initio quantum methods. 15 , 16 , 33 , 35 − 37 Major dissociative transformations of irradiated molecular systems (such as molecular topology changes, redistribution of atomic partial charges, or alteration of interatomic interactions) are simulated by means of MD with reactive force fields, particularly the reactive CHARMM (rCHARMM) force field 32 implemented in MBN Explorer.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

et al. 2023

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Irradiation-driven fragmentation and chemical transformations of molecular systems play a key role in nanofabrication processes where organometallic compounds break up due to the irradiation with focused particle beams. In this study, reactive molecular dynamics simulations have been performed to analyze the role of the molecular environment on the irradiation-induced fragmentation of molecular systems. As a case study, we consider the dissociative ionization of iron pentacarbonyl, Fe(CO) 5 , a widely used precursor molecule for focused electron beam-induced deposition. In connection to recent experiments, the irradiationinduced fragmentation dynamics of an isolated Fe(CO) 5 + molecule is studied and compared with that of Fe(CO) 5 + embedded into an argon cluster. The appearance energies of different fragments of isolated Fe(CO) 5+ agree with the recent experimental data. For Fe(CO) 5 + embedded into an argon cluster, the simulations reproduce the experimentally observed suppression of Fe(CO) 5 + fragmentation and provide an atomistic-level understanding of this effect. Understanding irradiation-driven fragmentation patterns for molecular systems in environments facilitates the advancement of atomistic models of irradiation-induced chemistry processes involving complex molecular systems.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

et al. 2023

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Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment

Solov’yov,

Verkhovtsev,

Mason

et al. 2024

Chem. Rev.

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This roadmap reviews the new, highly interdisciplinary research field studying the behavior of condensed matter systems exposed to radiation. The Review highlights several recent advances in the field and provides a roadmap for the development of the field over the next decade. Condensed matter systems exposed to radiation can be inorganic, organic, or biological, finite or infinite, composed of different molecular species or materials, exist in different phases, and operate under different thermodynamic conditions. Many of the key phenomena related to the behavior of irradiated systems are very similar and can be understood based on the same fundamental theoretical principles and computational approaches. The multiscale nature of such phenomena requires the quantitative description of the radiation-induced effects occurring at different spatial and temporal scales, ranging from the atomic to the macroscopic, and the interlinks between such descriptions. The multiscale nature of the effects and the similarity of their manifestation in systems of different origins necessarily bring together different disciplines, such as physics, chemistry, biology, materials science, nanoscience, and biomedical research, demonstrating the numerous interlinks and commonalities between them. This research field is highly relevant to many novel and emerging technologies and medical applications.

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Investigating electron-induced dissociation dynamics in the organometallic precursor Fe(CO)₅: a nonadiabatic molecular dynamics approach

Cui,

Zheng,

Gao

et al. 2024

J. Phys. D: Appl. Phys.

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This research employs excited states molecular dynamics simulations to explore the electron-induced dissociation behavior of Fe(CO)5 molecules, with the specific focus on electronic excitation. The study initiates with the detailed analysis of the molecule’s stable ground state structure. Subsequent simulations reveal distinctive dissociation patterns in various bonds, particularly noting the rapid dissociation of bonds between Fe and C1, Fe and C2, while those with Fe and C3 oscillate without complete dissociation. Emphasizing the influence of the transition from the highest occupied molecular orbital to the lowest unoccupied molecular orbital on reactivity, the investigation sheds light on the charge transfer phenomenon during dissociation through Bader analysis. Insights into transitions between excited and ground states are derived from the time evolution of the Kohn–Sham orbital. This study significantly contributes to understanding intricate dissociation mechanisms under electronic excitation, especially in molecules like Fe(CO)5 characterized by complex chemical bonds. Beyond theoretical exploration, the research holds practical significance for applications in nanomaterials, such as focused electron beam-induced deposition and the fabrication of nanoscale structures, enriching our comprehension of electronic-excitation-induced dissociation and advancing both theoretical understanding and practical applications in this field.

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Atomistic simulation of the FEBID-driven growth of iron-based nanostructures

Abstract: The growth of iron-containing nanostructures in the process of focused electron beam-induced deposition (FEBID) of Fe(CO)5 is studied by means of atomistic irradiation-driven molecular dynamics (IDMD) simulations. The geometrical characteristics...

Cited by 4 publications

References 57 publications

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment

Investigating electron-induced dissociation dynamics in the organometallic precursor Fe(CO)₅: a nonadiabatic molecular dynamics approach

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Atomistic simulation of the FEBID-driven growth of iron-based nanostructures

Abstract: The growth of iron-containing nanostructures in the process of focused electron beam-induced deposition (FEBID) of Fe(CO)5 is studied by means of atomistic irradiation-driven molecular dynamics (IDMD) simulations. The geometrical characteristics...

Cited by 4 publications

References 57 publications

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)5: A Reactive Molecular Dynamics Study

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)5: A Reactive Molecular Dynamics Study

Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment

Investigating electron-induced dissociation dynamics in the organometallic precursor Fe(CO)5: a nonadiabatic molecular dynamics approach

Contact Info

Product

Resources

About

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

Role of the Molecular Environment in Quenching the Irradiation-Driven Fragmentation of Fe(CO)₅: A Reactive Molecular Dynamics Study

Investigating electron-induced dissociation dynamics in the organometallic precursor Fe(CO)₅: a nonadiabatic molecular dynamics approach