Electrically driven cascaded photon emission in a single molecule

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F68378271%3A_____%2F25%3A00636951" target="_blank" >RIV/68378271:_____/25:00636951 - isvavai.cz</a>

Výsledek na webu

<a href="https://hdl.handle.net/11104/0367917" target="_blank" >https://hdl.handle.net/11104/0367917</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1103/PhysRevX.15.021072" target="_blank" >10.1103/PhysRevX.15.021072</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Electrically driven cascaded photon emission in a single molecule

Popis výsledku v původním jazyce

Controlling electrically stimulated quantum light sources (QLSs) is key for developing integrated and low-scale quantum devices. The underlying mechanisms leading to electrically driven quantum emission, however, are complex, as a large number of electronic states of the system can be involved and, thus, impact the emission dynamics. Here, we use a scanning tunneling microscope to electrically excite a model QLS, namely, a single ZnPc molecule, and disentangle the interplay of charge transfer and excited state formation. The luminescence spectra reveal two lines, associated to the emission of the neutral (exciton) and positively charged (trion) ZnPc, both exhibiting single-photon source behavior. In addition, we find a correlation between the charged and neutral emission, specifically, the signature of a photon cascade in which the radiative decay of the molecular trion is followed by the formation and decay of the exciton. By adjusting the charging vs discharging rate, we show that we can control these emission statistics. This generic strategy is further established by a comprehensive rate equation model comprising a variety of states that mediate excited state formation in the electrically driven single and cascaded photon emission process, revealing the complex internal dynamics of the molecular junction.

Název v anglickém jazyce

Electrically driven cascaded photon emission in a single molecule

Popis výsledku anglicky

Controlling electrically stimulated quantum light sources (QLSs) is key for developing integrated and low-scale quantum devices. The underlying mechanisms leading to electrically driven quantum emission, however, are complex, as a large number of electronic states of the system can be involved and, thus, impact the emission dynamics. Here, we use a scanning tunneling microscope to electrically excite a model QLS, namely, a single ZnPc molecule, and disentangle the interplay of charge transfer and excited state formation. The luminescence spectra reveal two lines, associated to the emission of the neutral (exciton) and positively charged (trion) ZnPc, both exhibiting single-photon source behavior. In addition, we find a correlation between the charged and neutral emission, specifically, the signature of a photon cascade in which the radiative decay of the molecular trion is followed by the formation and decay of the exciton. By adjusting the charging vs discharging rate, we show that we can control these emission statistics. This generic strategy is further established by a comprehensive rate equation model comprising a variety of states that mediate excited state formation in the electrically driven single and cascaded photon emission process, revealing the complex internal dynamics of the molecular junction.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Physical Review X

ISSN

2160-3308

e-ISSN

2160-3308

Svazek periodika

15

Číslo periodika v rámci svazku

2

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

20

Strana od-do

021072

Kód UT WoS článku

001512689900001

EID výsledku v databázi Scopus

2-s2.0-105007042200