| 000 | 02677 am a22003733u 4500 | ||
|---|---|---|---|
| 042 | _adc | ||
| 100 | 1 | 0 |
_aGillett, Alexander J. _eauthor _91393 |
| 700 | 1 | 0 |
_aPershin, Anton _eauthor _91394 |
| 700 | 1 | 0 |
_aPandya, Raj _eauthor _91395 |
| 700 | 1 | 0 |
_aFeldmann, Sascha _eauthor _91396 |
| 700 | 1 | 0 |
_aSneyd, Alexander J. _eauthor _91397 |
| 700 | 1 | 0 |
_aAlvertis, Antonios M. _eauthor _91398 |
| 700 | 1 | 0 |
_aEvans, Emrys W. _eauthor _91399 |
| 700 | 1 | 0 |
_aThomas, Tudor H. _eauthor _91400 |
| 700 | 1 | 0 |
_aCui, Lin-Song _eauthor _91401 |
| 700 | 1 | 0 |
_aDrummond, Bluebell H. _eauthor _91402 |
| 700 | 1 | 0 |
_aScholes, Gregory D. _eauthor _91403 |
| 700 | 1 | 0 |
_aOlivier, Yoann _eauthor _91404 |
| 700 | 1 | 0 |
_aRao, Akshay _eauthor _91405 |
| 700 | 1 | 0 |
_aFriend, Richard H. _eauthor _91406 |
| 700 | 1 | 0 |
_aBeljonne, David _eauthor _91407 |
| 245 | 0 | 0 | _aDielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters |
| 260 | _c2022-10. | ||
| 500 | _a/pmc/articles/PMC7613666/ | ||
| 500 | _a/pubmed/35927434 | ||
| 520 | _aThermally-activated delayed fluorescence (TADF) enables organic semiconductors with charge transfer (CT)-type excitons to convert dark triplet states into bright singlets via reverse intersystem crossing (rISC). However, thus far the contribution from the dielectric environment has received insufficient attention. Here, we study the role of the dielectric environment in a range of TADF materials with varying changes in dipole moment upon optical excitation. In dipolar emitters, we observe how environmental reorganisation after excitation triggers the full CT exciton formation, minimising the singlet-triplet energy gap, with the emergence of two (reactant-inactive) modes acting as a vibrational fingerprint of the CT product. In contrast, the dielectric environment plays a smaller role in less dipolar materials. The analysis of energy-time trajectories and their free-energy functions reveal that the dielectric environment significantly reduces the activation energy for rISC in dipolar TADF emitters, increasing the rISC rate by three orders of magnitude versus the isolated molecule. | ||
| 540 | _a | ||
| 540 | _ahttps://www.springernature.com/gp/open-research/policies/accepted-manuscript-termsUsers may view, print, copy, and download text and data-mine the content in such documents, for the purposes of academic research, subject always to the full Conditions of use: https://www.springernature.com/gp/open-research/policies/accepted-manuscript-terms | ||
| 546 | _aen | ||
| 690 | _aArticle | ||
| 655 | 7 |
_aText _2local |
|
| 786 | 0 | _nNat Mater | |
| 856 | 4 | 1 |
_uhttp://dx.doi.org/10.1038/s41563-022-01321-2 _zConnect to this object online. |
| 999 |
_c800 _d800 |
||