Title: Elucidating non-radiative decay in near-infrared lumiphores: Leveraging new design principles to develop a telecom band organic dye laser

Journal Article · · Chem
 [1];  [1];  [2];  [1];  [1];  [3]; ORCiD logo [1]
  1. Univ. of Chicago, IL (United States)
  2. Princeton Univ., NJ (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Organic near-infrared (NIR) lumiphores have been targeted for biological and technological applications; however, these dyes exhibit exponentially decreasing quantum yields with decreasing energy gaps. The accepted model of this phenomenon invokes C–H stretching modes as the dominant route of non-radiative energy dissipation. Reducing the number of these modes is a popular strategy for the design of bright NIR lumiphores, but quantitative experimental validation of this strategy is lacking. Here, we evaluate the role of C–H modes in non-radiative relaxation through isotopic labeling of a NIR-emitting complex. Measurements comparing relaxation between protonated and perdeuterated complexes indicate that C–H modes do not contribute significantly to non-radiative relaxation. We instead propose that skeletal modes may play a larger role and suggest that minimizing scaffold size is a promising route for bright NIR lumiphores. In conclusion, we demonstrate the promise of such strategies through the development of the reddest organic-based laser dye yet reported.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Dreyfus Teacher-Scholar Award; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; SC0019215
OSTI ID:
2569923
Journal Information:
Chem, Journal Name: Chem Journal Issue: 7 Vol. 10; ISSN 2451-9294
Publisher:
Cell PressCopyright Statement
Country of Publication:
United States
Language:
English

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