Above the Energy Gap Law: Heavy Chalcogenide Substitution in NIR II-Emissive Diradicaloid Qubits
Year: 2025
Type: article
Abstract: Near-infrared (NIR, 700-1700 nm)- and telecom (∼1260-1625 nm)-emissive molecules are good candidates for biological imaging and quantum sensing applications, respectively; however, bright low energy emission is rare due to exponentially increasing nonradiative decay rates in these regions, a phenomenon known as the energy gap law. Recent literature has emphasized the importance of minimizing skeletal modes to prevent increased nonradiative decay rates, but most organic lumiphores in these regions utilize large, conjugated scaffolds containing many CC modes. Here we report a compact, telecom-emissive scaffold, tetrathiafulvalene-2,3,6,7-tetraselenate, or TTFts, that displays remarkable air, water, and acid stability, exhibits record quantum yields and brightness values, and retains quantum coherence under ambient conditions. These properties are enabled through methodical selenium substitution, which bathochromically shifts emission while shifting skeletal vibrations to lower energies. This new scaffold validates heavy heteroatom substitution strategies and establishes a new class of bright telecom emitters and robust qubits.
Source: ACS Central Science
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: diamond
Funders: National Science Foundation, U.S. Department of Energy, 3M, University of Chicago, Westlake University, National Natural Science Foundation of China, Office of Science, Materials Research Science and Engineering Center, Harvard University, Division of Materials Research, Basic Energy Sciences, Army Research Office, Argonne National Laboratory
Awards: G102163711, G1055550527, G107546177, Materials Research Science and Engineering Centers, G1286251239, G1673814530, QUANTUM COMPUTING ALGORITHMS AND APPLICATIONS FOR COHERENT AND STRONGLY CORRELATED CHEMICAL SYSTEMS, QUANTUM COMPUTING ALGORITHMS AND APPLICATIONS FOR COHERENT AND STRONGLY CORRELATED CHEMICAL SYSTEMS, G2287611682, G262962599, G2867976162, G2875663643, G2916140176, G3122338967, G3589692066, G4230073126, G426311843, G4644544412, G498139845, G513797252, G5387317844, G6599444349, G6848031779, G6918803902, G6991494858, G7452299184, G7583137537, G837711380, G8671621397, G880751848, G969889393, G993149817
OpenAlex ID: W4415664872