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              <p>The present investigation describes an original structure–reactivity relationship within a series of type II photoinitiators designed on the basis of a multibranched molecular engineering strategy. Each photoinitiator indeed incorporates a triphenylamine subunit decorated with a combination of para-substituents, implying anisole or thioanisole as π-conjugated donor groups and multiple reactive ketones as electron-acceptor functions. Interestingly, we demonstrate that the photoinitiating efficiency of such multipolar derivatives is mainly modulated by a solvent-mediated interplay between intersystem crossing and intramolecular charge transfer processes at the excited singlet state. Such a balancing mechanism drastically regulates the population of highly reactive excited triplet species in such a manner that the photoinitiation performance of the dyes can be enhanced by more than 1 order of magnitude within the series. Taking advantage of this amplified photoreactivity, we illustrated the versatile application potential of the best-performing photoinitiating prototype, which was both employed both in a rapid two-dimensional (2D) photopatterning process through liquid crystal display (LCD) image projection and in three-dimensional (3D) micro-optics fabrication at the surface of an optical fiber.</p>
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        <org type="institution" xml:id="struct-420786" status="VALID">
          <idno type="IdRef">028021037</idno>
          <idno type="ISNI">0000000121497878</idno>
          <idno type="ROR">https://ror.org/05ggc9x40</idno>
          <orgName>Université Paris-Est Créteil Val-de-Marne - Paris 12</orgName>
          <orgName type="acronym">UPEC UP12</orgName>
          <date type="start">1970-01-01</date>
          <desc>
            <address>
              <addrLine>61 avenue du Général de Gaulle - 94010 Créteil cedex</addrLine>
              <country key="FR"/>
            </address>
            <ref type="url">http://www.u-pec.fr/</ref>
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