Ultrafast nonradiative bright-to-dark exciton relaxation facilitated by excitonic effects at <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>As</mml:mi> <mml:mo>/</mml:mo> <mml:msub> <mml:mi>SnS</mml:mi> <mml:mn>2</mml:mn

Momentum-forbidden dark excitons with suppressed radiative recombination and extended lifetimes are promising for optoelectronic applications. However, the relaxation mechanism from bright to dark excitons, as well as the influence of excitonic effects and temperature, remains unclear in van der Waals heterostructures. Here, the bright-dark exciton transitions of As/${\mathrm{SnS}}_{2}$ heterostructures are investigated through nonadiabatic molecular dynamics combined with the $\mathit{GW}$ plus real-time Bethe-Salpeter equation. We discover that high temperature induces phonon excitation to facilitate exciton relaxation, but the large bright-dark exciton energy difference induced by interfacial interaction limits the phonon scattering efficiency. In contrast, the electron-hole Coulomb interactions from excitonic effects exhibit strong nonadiabatic coupling and provide additional relaxation channels that dominate the ultrafast (\ensuremath{\sim}200 fs) bright-dark exciton transitions at different temperatures and stacking configurations. Neglecting the excitonic effects results in much slower transitions, with the maximum difference in transition time reaching a factor of $17\phantom{\rule{0.16em}{0ex}}292$. The resulting dark excitons exhibit long nonradiative lifetimes (\ensuremath{\sim}50 ps at room temperature). The proposed physical mechanism is crucial for understanding the formation of dark excitons and for designing optoelectronic devices with long-lived excitonic states in van der Waals heterostructures.

Authors

Institutions

Publication Details

Journal
Physical review. B./Physical review. B
Published
2025-11-06
DOI
https://doi.org/10.1103/pgcl-cqs3
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
0.00
Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Ultrafast nonradiative bright-to-dark exciton relaxation facilitated by excitonic effects at <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>As</mml:mi> <mml:mo>/</mml:mo> <mml:msub> <mml:mi>SnS</mml:mi> <mml:mn>2</mml:mn

Zuoyin Liu, Aijun Du, Zhenyi Jiang, Yanming Lin
Physical review. B./Physical review. B
2D Materials and Applications
article

Ultrafast nonradiative bright-to-dark exciton relaxation facilitated by excitonic effects at <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>As</mml:mi> <mml:mo>/</mml:mo> <mml:msub> <mml:mi>SnS</mml:mi> <mml:mn>2</mml:mn

Zuoyin Liu, Aijun Du, Zhenyi Jiang, Yanming Lin
article en

Abstract

Momentum-forbidden dark excitons with suppressed radiative recombination and extended lifetimes are promising for optoelectronic applications. However, the relaxation mechanism from bright to dark excitons, as well as the influence of excitonic effects and temperature, remains unclear in van der Waals heterostructures. Here, the bright-dark exciton transitions of As/${\mathrm{SnS}}_{2}$ heterostructures are investigated through nonadiabatic molecular dynamics combined with the $\mathit{GW}$ plus real-time Bethe-Salpeter equation. We discover that high temperature induces phonon excitation to facilitate exciton relaxation, but the large bright-dark exciton energy difference induced by interfacial interaction limits the phonon scattering efficiency. In contrast, the electron-hole Coulomb interactions from excitonic effects exhibit strong nonadiabatic coupling and provide additional relaxation channels that dominate the ultrafast (\ensuremath{\sim}200 fs) bright-dark exciton transitions at different temperatures and stacking configurations. Neglecting the excitonic effects results in much slower transitions, with the maximum difference in transition time reaching a factor of $17\phantom{\rule{0.16em}{0ex}}292$. The resulting dark excitons exhibit long nonradiative lifetimes (\ensuremath{\sim}50 ps at room temperature). The proposed physical mechanism is crucial for understanding the formation of dark excitons and for designing optoelectronic devices with long-lived excitonic states in van der Waals heterostructures.

Physical review. B./Physical review. BVol. 112(19)
Queensland University of Technology (AU), Northwest University (CN), Institute of Modern Physics (CN)
Openalex Percentile: Top 74%
2D Materials and Applications
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.