Real-Time Electron Dynamics Study of Plasmon-Mediated Photocatalysis on an Icosahedral Al13-1 Nanocluster
Nitrogen bond dissociation is one of the important steps in the Haber-Bosch process, where N2 is catalytically converted to NH3; however, the dissociation of the nitrogen triple bond is difficult to achieve. In this study, we investigate the possibility of nitrogen activation using plasmonic excitation of an icosahedral aluminum nanocluster. Real-time time-dependent density functional theory is employed to study the electron dynamics of the Al13-1 and [Al13N2]-1 systems. Step and trapezoidal electric fields with field strengths of 0.001 and 0.01 au and different polarization directions are applied to the systems, and the electron dynamics are analyzed. Because the occupation of nitrogen antibonding orbitals could potentially activate the N-N bond, we investigated the single-particle electronic transitions corresponding to an excitation from an occupied (O) to virtual (V) molecular orbitals (POV) of [Al13N2]-1. We found that N2 antibonding orbitals are more likely to become populated with stronger fields and also by using off-resonance fields.
Medienart: |
E-Artikel |
---|
Erscheinungsjahr: |
2021 |
---|---|
Erschienen: |
2021 |
Enthalten in: |
Zur Gesamtaufnahme - volume:125 |
---|---|
Enthalten in: |
The journal of physical chemistry. A - 125(2021), 22 vom: 10. Juni, Seite 4847-4860 |
Sprache: |
Englisch |
---|
Beteiligte Personen: |
Pandeya, Pratima [VerfasserIn] |
---|
Links: |
---|
Themen: |
---|
Anmerkungen: |
Date Completed 17.06.2021 Date Revised 17.06.2021 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
---|
doi: |
10.1021/acs.jpca.1c02924 |
---|
funding: |
|
---|---|
Förderinstitution / Projekttitel: |
|
PPN (Katalog-ID): |
NLM325969760 |
---|
LEADER | 01000naa a22002652 4500 | ||
---|---|---|---|
001 | NLM325969760 | ||
003 | DE-627 | ||
005 | 20231225193556.0 | ||
007 | cr uuu---uuuuu | ||
008 | 231225s2021 xx |||||o 00| ||eng c | ||
024 | 7 | |a 10.1021/acs.jpca.1c02924 |2 doi | |
028 | 5 | 2 | |a pubmed24n1086.xml |
035 | |a (DE-627)NLM325969760 | ||
035 | |a (NLM)34048246 | ||
040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
041 | |a eng | ||
100 | 1 | |a Pandeya, Pratima |e verfasserin |4 aut | |
245 | 1 | 0 | |a Real-Time Electron Dynamics Study of Plasmon-Mediated Photocatalysis on an Icosahedral Al13-1 Nanocluster |
264 | 1 | |c 2021 | |
336 | |a Text |b txt |2 rdacontent | ||
337 | |a ƒaComputermedien |b c |2 rdamedia | ||
338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
500 | |a Date Completed 17.06.2021 | ||
500 | |a Date Revised 17.06.2021 | ||
500 | |a published: Print-Electronic | ||
500 | |a Citation Status PubMed-not-MEDLINE | ||
520 | |a Nitrogen bond dissociation is one of the important steps in the Haber-Bosch process, where N2 is catalytically converted to NH3; however, the dissociation of the nitrogen triple bond is difficult to achieve. In this study, we investigate the possibility of nitrogen activation using plasmonic excitation of an icosahedral aluminum nanocluster. Real-time time-dependent density functional theory is employed to study the electron dynamics of the Al13-1 and [Al13N2]-1 systems. Step and trapezoidal electric fields with field strengths of 0.001 and 0.01 au and different polarization directions are applied to the systems, and the electron dynamics are analyzed. Because the occupation of nitrogen antibonding orbitals could potentially activate the N-N bond, we investigated the single-particle electronic transitions corresponding to an excitation from an occupied (O) to virtual (V) molecular orbitals (POV) of [Al13N2]-1. We found that N2 antibonding orbitals are more likely to become populated with stronger fields and also by using off-resonance fields | ||
650 | 4 | |a Journal Article | |
700 | 1 | |a Aikens, Christine M |e verfasserin |4 aut | |
773 | 0 | 8 | |i Enthalten in |t The journal of physical chemistry. A |d 1997 |g 125(2021), 22 vom: 10. Juni, Seite 4847-4860 |w (DE-627)NLM098261479 |x 1520-5215 |7 nnns |
773 | 1 | 8 | |g volume:125 |g year:2021 |g number:22 |g day:10 |g month:06 |g pages:4847-4860 |
856 | 4 | 0 | |u http://dx.doi.org/10.1021/acs.jpca.1c02924 |3 Volltext |
912 | |a GBV_USEFLAG_A | ||
912 | |a GBV_NLM | ||
951 | |a AR | ||
952 | |d 125 |j 2021 |e 22 |b 10 |c 06 |h 4847-4860 |