Unveiling the role of upper excited electronic states in the photochemistry and laser performance of anti-B18H22

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60076658%3A12310%2F20%3A43901368" target="_blank" >RIV/60076658:12310/20:43901368 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61388980:_____/20:00532242

Výsledek na webu

<a href="https://pubs.rsc.org/en/content/articlelanding/2020/TC/D0TC02309D#!divAbstract" target="_blank" >https://pubs.rsc.org/en/content/articlelanding/2020/TC/D0TC02309D#!divAbstract</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/d0tc02309d" target="_blank" >10.1039/d0tc02309d</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Unveiling the role of upper excited electronic states in the photochemistry and laser performance of anti-B18H22

Popis výsledku v původním jazyce

In the search for innovative new light sources, the discovery that solutions of the boron hydride anti-B18H22 generate photostable blue laser emission stands out in its significance as the first laser borane. Surprisingly, though, the laser performance of anti-B18H22 (similar to 10% efficiency) does not match the expectations based on its exceptional photophysical properties (Phi(f) = 0.97 and high photostability). To understand this contradiction, we herein present an investigation into the upper excited states of the anti-B18H22 photophysical system, which we suggest to be the most relevant factor to its laser performance. The use of computational quantum chemistry, laser and UV-vis spectroscopy, NMR spectroscopy, and mass spectrometry unveil the role of the upper excited states on the laser performance of anti-B18H22, showing that efficient excited state absorption (ESA) leads to the population of these states, and results not only in the loss of laser efficiency, but also in the activation of chemically reactive relaxation pathways and the formation of photochemically produced novel molecular species. The likely composition of these photoproducts, formed upon prolonged high intensity laser irradiation, is inferred from their molecular masses, NMR properties, and calculated natural orbitals. Together, these results are of key importance to the complete understanding of the anti-B18H22 photophysical system and provide valuable information to chemists and laser physicists working to mitigate deficiencies and enhance the performance of the next generation of borane lasers and borane-based photoactive materials.

Název v anglickém jazyce

Unveiling the role of upper excited electronic states in the photochemistry and laser performance of anti-B18H22

Popis výsledku anglicky

In the search for innovative new light sources, the discovery that solutions of the boron hydride anti-B18H22 generate photostable blue laser emission stands out in its significance as the first laser borane. Surprisingly, though, the laser performance of anti-B18H22 (similar to 10% efficiency) does not match the expectations based on its exceptional photophysical properties (Phi(f) = 0.97 and high photostability). To understand this contradiction, we herein present an investigation into the upper excited states of the anti-B18H22 photophysical system, which we suggest to be the most relevant factor to its laser performance. The use of computational quantum chemistry, laser and UV-vis spectroscopy, NMR spectroscopy, and mass spectrometry unveil the role of the upper excited states on the laser performance of anti-B18H22, showing that efficient excited state absorption (ESA) leads to the population of these states, and results not only in the loss of laser efficiency, but also in the activation of chemically reactive relaxation pathways and the formation of photochemically produced novel molecular species. The likely composition of these photoproducts, formed upon prolonged high intensity laser irradiation, is inferred from their molecular masses, NMR properties, and calculated natural orbitals. Together, these results are of key importance to the complete understanding of the anti-B18H22 photophysical system and provide valuable information to chemists and laser physicists working to mitigate deficiencies and enhance the performance of the next generation of borane lasers and borane-based photoactive materials.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

<a href="/cs/project/GA18-20286S" target="_blank" >GA18-20286S: Klastry hydridů boru pro lasery: Pochopení chemických a strukturálních faktorů, které určují fotofyziku anti-B18H22 a jejích derivátů</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2020

Kód důvěrnosti údajů

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

Název periodika

Journal of Materials Chemistry C

ISSN

2050-7526

e-ISSN

—

Svazek periodika

8

Číslo periodika v rámci svazku

37

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

13

Strana od-do

12806-12818

Kód UT WoS článku

000574416900037

EID výsledku v databázi Scopus

2-s2.0-85094957968