arXiv subjects

Cristián G. Sánchez

Publications and source records attributed to Cristián G. Sánchez.

10 recordsLinked to original sources

arXiv2026

Dissipation effects in the Su-Schrieffer-Heeger model coupled to a metallic environment

We theoretically study the electronic and lattice properties of a trans-polyacetylene (tPA) molecule deposited on top of a metallic substrate at equilibrium. We describe the system using a modified Su-Schrieffer-Heeger (SSH) model generalized to incorporate the effects of a metallic environment, represented by independent one-dimensional semi-infinite chains coupled to each site of the SSH chain (i.e., ``local bath approximation"). We focus on the zero-temperature case and obtain the physical properties of an $N$-site tPA chain deposited on a metallic surface by minimizing its total ground-state energy (i.e., electronic plus lattice degrees of freedom) as a function of the $N$ lattice-site positions. Interestingly, in the case of a homogeneous metallic substrate, where all coupling parameters are assumed identical, the SSH chain undergoes a zero-temperature insulator-to-metal transition as the coupling parameter $γ_0$ reaches a critical value where the Peierls dimerization is fully suppressed and the system becomes metallic. In addition, our model can be generalized to describe inhomogeneous situations where the substrate contains metallic and insulating regions, as usually occurs in realistic experiments containing accidentally oxidized decoupling layers. In this case, our results predict the occurrence of local nucleation of the metalized or the Peierls-dimerized phase within the same tPA molecule, depending on whether the surface directly beneath the molecule is metallic or insulating, respectively. We finally discuss the relevance of our findings for both the correct interpretation of existing tPA/Cu(110) experiments, as well as for their possible utility in the design of novel organic nanoelectronic devices.

cond-mat.mes-hall↗

arXiv2025

Towards electrical domain-wall control in polyacetylene-based electronic nanodevices

We theoretically propose a polymer-based nano-device consisting of a single trans-polyacetylene (tPA) molecule capacitively coupled to external voltage gates. We model the integrated device using a Su-Schrieffer-Heeger (SSH)-like Hamiltonian, and we demonstrate the emergence of localized domain walls (DWs) with quantized charges (i.e., soliton excitations) localized at the gates. Interestingly, by increasing the applied voltage, multiple discrete charges can be accumulated, which may be useful for potential technological applications. Exploiting the topological character of the solitonic excitations of tPA, this device can be considered as an organic-based quantum dot with a very large and robust quantized charge.

cond-mat.mes-hall↗

arXiv2023

Stability of moving solitons in trans-polyacetylene in an electric field

In this work we study the dynamics and stability of charged solitons in trans-polyacetylene (tPA), and revisit the issue of the stability of these non-linear excitations under the effect of an external electric field applied parallel to the polymer. Using the formalism of the Su-Schrieffer-Heeger (SSH) model, we solve the coupled dynamical equations for electrons and classical nuclei at the mean-field level and in the regime of low external electric field $E$, where the dynamics of the moving soliton is adiabatic. Analyzing observable quantities in real space and frequency space, we identify the microscopic mechanisms triggering the dynamical instabilities of the soliton. In addition, we put forward the definition of a proper quantitative measure of its stability, an issue which to the best of our knowledge has remained an open question. Besides its intrinsic interest from the fundamental point of view, our work might be relevant for the design of novel organic electronic devices based on soliton-mediated transport.

cond-mat.mes-hall↗

arXiv2022

Data-driven approach for benchmarking DFTB-approximate excited state methods

In this work we propose a chemically-informed data-driven approach to benchmark the approximate density-functional tight-binding (DFTB) excited state (ES) methods that are currently available within the DFTB+ suite. By taking advantage of the large volume of low-detail ES-data in the machine learning (ML) dataset, QM8, we were able to extract valuable insights regarding the limitations of the benchmarked methods in terms of the approximations made to the parent formalism, density-functional theory (DFT), while providing recommendations on how to overcome them. For this benchmark, we compared the first singlet-singlet vertical excitation energies ($E_1$) predicted by the DFTB-approximate methods with predictions of less approximate methods from the reference ML-dataset. For the nearly 21,800 organic molecules in the GDB-8 chemical space, we were able to identify clear trends in the $E_1$ prediction error distributions, with respect to second-order approximate coupled cluster (CC2), showing a strong dependence on chemical identity.

physics.chem-ph↗

arXiv2022

Dynamical evolution of the Schottky barrier as a determinant contribution to electron-hole pair stabilization and photocatalysis of plasmon-induced hot carriers

The harnessing of plasmon-induced hot carriers promises to open new avenues for the development of clean energies and chemical catalysis. The extraction of carriers before thermalization and recombination is of primordial importance to obtain appealing conversion yields. Here, hot carrier injection in the paradigmatic Au-TiO$_{2}$ system is studied by means of electronic and electron-ion dynamics. Our results show that pure electronic features (without considering many-body interactions or dissipation to the environment) contribute to the electron-hole separation stability. These results reveal the existence of a dynamic contribution to the interfacial potential barrier (Schottky barrier) that arises at the charge injection pace, impeding electronic back transfer. Furthermore, we show that this charge separation stabilization provides the time needed for the charge to leak to capping molecules placed over the TiO$_{2}$ surface triggering a coherent bond oscillation that will lead to a photocatalytic dissociation. We expect that our results will add new perspectives to the interpretation of the already detected long-lived hot carrier lifetimes, their catalytical effect, and concomitantly to their technological applications.

cond-mat.mes-hall↗

arXiv2022

Fano resonance and incoherent interlayer excitons in molecular van der Waals heterostructures

Complex van der Waals heterostructures from layered molecular stacks are promising optoelectronic materials offering means to efficient, modular charge separation and collection layers. The effect of stacking in the electrodynamics of such hybrid organic-inorganic two-dimensional materials remains largely unexplored, whereby molecular scale engineering could lead to advanced optical phenomena. For instance, tunable Fano engineering could make possible on-demand transparent conducting layers or photoactive elements, and passive cooling. We employ an adapted Gersten-Nitzan model and real time time-dependent density functional tight-binding to study the optoelectronics of self-assembled monolayers on graphene nanoribbons. We find Fano resonances that cause electromagnetic induced opacity and transparency, and reveal an additional incoherent process leading to interlayer exciton formation with a characteristic charge transfer rate. These results showcase hybrid van der Waals heterostructures as paradigmatic 2D optoelectronic stacks, featuring tunable Fano optics and unconventional charge transfer channels.

cond-mat.mes-hall↗

arXiv2020

A real-time time-dependent density functional tight-binding implementation for semiclassical excited state electron-nuclear dynamics and pump-probe spectroscopy simulations

The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the power of the approximate DFTB method with the semiclassical Ehrenfest method for nuclear-electron dynamics we have achieved a real-time time-dependent DFTB (TD-DFTB) implementation that fits such requirements. In addition to enabling the study of nuclear motion effects in photoinduced charge transfer processes, our code adds novel features to the realm of static and time-resolved computational spectroscopies. In particular, the optical properties of periodic materials such as graphene nanoribbons or the use of corrections such as the "LDA+U" and "pseudo SIC" methods to improve the optical properties in some systems, can now be handled at the TD-DFTB level. Moreover, the simulation of fully-atomistic time-resolved transient absorption spectra and impulsive vibrational spectra can now be achieved within reasonable computing time, owing to the good performance of the implementation and a parallel simulation protocol. Its application to the study of UV/visible light-induced vibrational coherences in molecules is demonstrated and opens a new door into the mechanisms of non-equilibrium ultrafast phenomena in countless materials with relevant applications.

physics.comp-ph↗

arXiv2019

Driven Liouville-von Neumann Equation for Quantum Transport and Multiple-Probe Green's Functions

The so called Driven Liouville-von Neumann equation is a dynamical formulation to simulate a voltage bias across a molecular system and to model a time-dependent current in a grand-canonical framework. This approach introduces a damping term in the equation of motion that drives the charge to a reference, out of equilibrium density. Originally proposed by Horsfield and co-workers, further work on this scheme has led to different coexisting versions of this equation. On the other hand, the multiple-probe scheme devised by Todorov and collaborators, known as the hairy-probes method, is a formal treatment based on Green's functions that allows to fix the electrochemical potentials in two regions of an open quantum system. In this article, the equations of motion of the hairy probes formalism are rewritten to show that, under certain conditions, they can assume the same algebraic structure as the Driven Liouville-von Neumann equation in the form proposed by Morzan et al. [J. Chem. Phys. 2017, 146, 044110]. In this way, a new formal ground is provided for the latter, identifying the origin of every term. The performance of the different methods are explored using tight-binding time-dependent simulations in three trial structures, designated as ballistic, disordered, and resonant models. In the context of first-principles Hamiltonians the Driven Liouville-von Neumann approach is of special interest, because it does not require the calculation of Green's functions. Hence, the effects of replacing the reference density based on the Green's function by one obtained from an applied field are investigated, to gain a deeper understanding of the limitations and the range of applicability of the Driven Liouville-von Neumann equation.

cond-mat.mes-hall↗

arXiv2016

Optical Properties of Graphene Nanoflakes: Shape Matters

In recent years there has been significant debate on whether the edge type of graphene nanoflakes (GNF) or graphene quantum dots (GQD) are relevant for their electronic structure, thermal stability and optical properties. Using computer simulations, we have proven that there is a fundamental difference in the calculated absorption spectra between samples of the same shape, similar size but different edge type, namely, armchair or zigzag edges. These can be explained by the presence of electronic structures near the Fermi level which are localized on the edges. These features are also evident from the dependence of band gap on the GNF size, which shows three very distinct trends for different shapes and edge geometries.

cond-mat.mes-hall↗

arXiv2015

Full quantum dynamics of the electronic coupling between photosynthetic pigments

From studying the time evolution of the single electron density matrix within a density functional tight-binding formalism we study in a fully atomistic picture the electronic excitation transfer between two photosynthetic pigments in real time. This time-dependent quantum dynamics is based on fully atomistic structural models of the photosynthetic pigment. We analyze the dependence of the electronic excitation transfer with distance and orientation between photosynthetic pigments. We compare the results obtained from full quantum dynamics with analytical ones, based on a two level system model were the interaction between the pigments is dipolar. We observed that even when the distance of the photosynthetic pigment is about $30$ Å the deviation of the dipolarity is of about $15$ percent.

physics.chem-ph↗