Laser-Controlled Charge Transfer in a Two-Dimensional Organic/Inorganic Optical Coherent Nanojunction

TL;DR

This study uses first-principles simulations to explore how laser pulses induce ultrafast charge transfer in a 2D MoSe2/pyrene nanojunction, revealing nonlinear behavior and the potential for ultrafast optoelectronic devices.

Contribution

It demonstrates the nonlinear charge transfer dynamics in a 2D organic/inorganic nanojunction under laser excitation, highlighting the role of Pauli blocking and multi-photon absorption.

Findings

Charge transfer direction reverses at high laser intensities.

Pauli blocking saturates electronic states beyond 200 GW/cm².

Multi-photon absorption influences charge dynamics.

Abstract

Understanding the fundamental mechanisms ruling laser-induced coherent charge transfer in hybrid organic/inorganic interfaces is of paramount importance to exploit these systems in next-generation opto-electronic applications. In a first-principles work based on real-time time-dependent density-functional theory, we investigate the ultrafast charge-carrier dynamics of a prototypical two-dimensional vertical nanojunction formed by a MoSe$_2$ monolayer with adsorbed pyrene molecules. The response of the system to the incident pulse, set in resonance with the frequency of the lowest-energy transition in the physisorbed moieties, is clearly nonlinear. Under weak pulses, charge transfer occurs from the molecules to the monolayer while for intensities higher than 1000 GW/cm$^{2}$, the direction of charge transfer is reverted, with electrons being transferred from MoSe$_2$ to pyrene. This finding is explained by Pauli blocking: laser-induced (de)population of (valence) conduction states saturates for intensities beyond 200 GW/cm$^{2}$. Evidence of multi-photon absorption is also provided by our results. A thorough analysis of electronic current density, excitation energy, and number of excited electrons supports the proposed rationale and suggests the possibility to create an inorganic/organic coherent optical nanojunction for ultrafast electronics.