期刊
NANO LETTERS
卷 9, 期 8, 页码 2820-2824出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl803717g
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资金
- EU [NMP4-CT-2004-500 19]
- FP7 ETSF 13 e-Infrastructure [211956]
- Belgian Interuniversity Attraction Poles Program [P6/42]
- Communaute Francaise de Belgique [ARC 07/12-003]
- Region wallone (WALL-ETSF)
Within the Tamm-Dancoff approximation, ab initio approaches describe excitons as packets of electron-hole pairs propagating only forward in time. However, we show that in nanoscale materials excitons and plasmons hybridize, creating exciton-plasmon states where the electron-hole pairs oscillate back and forth in time. Then, as exemplified by the trans-azobenzene molecule and the carbon nanotubes, the Tamm-Dancoff approximation yields errors larger than the accuracy claimed in ab initio calculations. Instead, we propose a general and efficient approach that avoids the Tamm-Dancoff approximation, correctly describes excitons, plasmons, and exciton-plasmon states, and provides a good agreement with experimental results.
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