Nanocrystal Assemblies: Current Advances and Open Problems

ACS Nano, Год журнала: 2024, Номер 18(23), С. 14791 - 14840

Опубликована: Май 30, 2024

We explore the potential of nanocrystals (a term used equivalently to nanoparticles) as building blocks for nanomaterials, and current advances open challenges fundamental science developments applications. Nanocrystal assemblies are inherently multiscale, generation revolutionary material properties requires a precise understanding relationship between structure function, former being determined by classical effects latter often quantum effects. With an emphasis on theory computation, we discuss that hamper assembly strategies what extent nanocrystal represent thermodynamic equilibrium or kinetically trapped metastable states. also examine dynamic optimization protocols. Finally, promising functions examples their realization with assemblies.

Язык: Английский

---

Theory and modeling of light-matter interactions in chemistry: current and future

Physical Chemistry Chemical Physics, Год журнала: 2023, Номер 25(46), С. 31554 - 31577

Опубликована: Янв. 1, 2023

Light-matter interaction not only plays an instrumental role in characterizing materials' properties via various spectroscopic techniques but also provides a general strategy to manipulate material the design of novel nanostructures. This perspective summarizes recent theoretical advances modeling light-matter interactions chemistry, mainly focusing on plasmon and polariton chemistry. The former utilizes highly localized photon, plasmonic hot electrons, local heat drive chemical reactions. In contrast, chemistry modifies potential energy curvatures bare electronic systems, hence their forming hybrid states, so-called polaritons. starts with basic background interactions, molecular quantum electrodynamics theory, challenges Then, are described, future directions toward multiscale simulations interaction-mediated discussed.

Язык: Английский

---

Nuclear-Electronic Orbital Quantum Dynamics of Plasmon-Driven H₂ Photodissociation

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(33), С. 18210 - 18214

Опубликована: Авг. 9, 2023

Leveraging localized surface plasmon resonances of metal nanoparticles to trigger chemical reactions is a promising approach for heterogeneous catalysis. First-principles modeling such processes challenging due the large number electrons and electronic excited states as well significance nuclear quantum effects when hydrogen involved. Herein, nonadiabatic nuclear-electronic dynamics plasmon-induced H2 photodissociation near an Al13- cluster simulated with real-time orbital time-dependent density functional theory (RT-NEO-TDDFT). This propagates nonequilibrium both protons. The plasmonic oscillations are shown inject hot into antibonding H2, thereby inducing dissociation. mechanical treatment nuclei leads faster slightly larger isotope effects. Analysis suggests that these findings stem from enhanced excited-state coupling between mode proton delocalization or zero-point energy Given low computational overhead including RT-NEO-TDDFT approach, this work paves way simulating in other systems.

Язык: Английский

---

Laser pulse induced second- and third-harmonic generation of gold nanorods with real-time time-dependent density functional tight binding (RT-TDDFTB) method

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(4)

Опубликована: Июль 23, 2024

In this study, we investigate second- and third-harmonic generation processes in Au nanorod systems using the real-time time-dependent density functional tight binding method. Our study focuses on computation of nonlinear signals based time dependent dipole response induced by linearly polarized laser pulses interacting with nanoparticles. We systematically explore influence various parameters, including pump intensity, duration, frequency, polarization directions, harmonic generation. demonstrate all results dimer arranged end-to-end configurations, disrupting spatial symmetry regular single is crucial for second-harmonic processes. Furthermore, impact lengths, which lead to variable plasmon energies, generation, estimates polarizabilities hyper-polarizabilities are provided.

Язык: Английский

---

Multipodal Au–C grafting of calix[4]arene molecules on gold nanorods

Chemical Science, Год журнала: 2024, Номер 15(36), С. 14677 - 14684

Опубликована: Янв. 1, 2024

Coupled experimental and computational characterizations establish the successful multipodal grafting of calix[4]arene macrocycles onto gold nanorods leading to robust functionalizable nanoobjects.

Язык: Английский

---

Mechanisms of Electron Transfer between Metal Clusters and Molecules in Plasmonic Junctions

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Апрель 2, 2025

Surface plasmons can localize the optical field and energy at nanoscale, significantly enhancing various light-matter interactions, such as in photocatalysis. The hot electrons generated by plasmon decay play a crucial role driving chemical reactions. To better understand mechanisms behind electron transfer, we have developed polarizability bond model to visualize how transfer influences polarization. In this study, examine molecule-metal coupled systems, where molecules of varying dimensions are embedded between metal clusters. Our findings show that is enhanced when molecular component directly excited. efficiency decreases cavity gap widens. Distinct behaviors observed across different systems with most pronounced enhancement occurring one-dimensional Further analysis reveals atoms first second layers clusters critical facilitating interfacial Intramolecular polarization particularly strong excitation originates from component, bonds near center or those aligned near-field more easily polarized excitation. This study atomic-level provides theoretical basis for optimizing plasmon-mediated catalytic

Язык: Английский

---

Integrative plasmonics: optical multi-effects and acousto-electric-thermal fusion for biosensing, energy conversion, and photonic circuits

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review traces the evolution from classical to integrative plasmonics, detailing optical multi-effects of plasmons and their acousto-optic-electric-thermal fusion. It discusses key integration mechanisms, applications, future prospects.

Язык: Английский

---

Plasmon-Enhanced Spectroscopy and Photocatalysis

Опубликована: Янв. 1, 2024

Язык: Английский

---

Real-Time Formulation of Atomistic Electromagnetic Models for Plasmonics

The Journal of Physical Chemistry C, Год журнала: 2024, Номер 128(41), С. 17513 - 17525

Опубликована: Окт. 4, 2024

Язык: Английский

---

Identifying Differences between Semiclassical and Full-Quantum Descriptions of Plexcitons

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(37), С. 9326 - 9334

Опубликована: Сен. 5, 2024

Strong light-matter coupling between molecules and plasmonic nanoparticles gives rise to new hybrid eigenstates of the coupled system, commonly referred as polaritons or, more precisely, plexcitons. Over past decade, it has been amply shown that molecular electron dynamics photophysics can be drastically affected by such interactions, thus paving way for light-induced control excited state properties reactivity. Here, combining ab initio description classical or quantum modeling arbitrarily shaped nanostructures within stochastic Schrödinger equation, we present two approaches, one semiclassical full-quantum, follow in real time electronic plexcitons while realistically taking dissipative losses into account. The full-quantum theory is compared with analogue under different interaction regimes, showing (numerically theoretically) even weak-field weak-coupling limit a small-yet-observable difference arises.

Язык: Английский

---