Molecular Supracence Resolving Eight Colors in 300‐nm Width: Unprecedented Spectral Resolution

Abstract

Monitoring multiple molecular probes simultaneously establishes their correlations and reveals the holistic mechanism. Current fluorescence imaging, however, is limited to about four colors because of typically circa 100-nm spectral width. Herein, we show that molecular supracence imparts superior spectral resolution, resolving eight colors in 300-nm width, about 37.5-nm per color. A recently discovered lightmolecule interacting phenomenon, supracence only measures molecular emission above its excitation energy due to entanglement between atomic quantum system and electronic quantum system. As such, supracence takes advantage of sharp spectral edge of a single pathway and excitation specificity to produce narrow bands, whereas fluorescence has to deal with multiple pathways spilling out low-energy long tail, that causes poor resolution. Thus, supracence enables myriad innovative molecular spectroscopy and microscopic imaging with profound impact broadly.

Full-Quantum Treatment of Molecular Systems Confirms Novel Supracence Photonic Properties

“…In fact, when both fluorescence and supracence are converging to the 0→0 position from opposite directions, the emission responds with maximizing intensity ( Figure 6 D). Corollary to these observations is that both supracence and fluorescence are exciting into the same 0→0 transition as proved earlier using the full quantum model [ 19 , 20 ], in which electrons and atoms are treated as two sub-quantum systems or dual quantum systems. Nevertheless, how does low-energy light excite into the higher 0→0 electro-optical transition to create high-energy supracence?…”

“…When photoexcitation occurs in bond-stretched structures (Δ R > 0; far from equilibrium and lower transition energy) and subsequent relaxation brings the molecule to near-equilibrium structures for emission (Δ R ≈ 0 and higher transition energy), the molecule will emit a photon with more energy than that absorbed ( Figure 9 E). This is supracence [ 19 , 20 ]. Considering the photon and the molecule as a thermodynamic system before absorption ( E A , A A , P A ) or after emission ( E E , A E , P E ) leads to energy conservation, i.e., E A + A A + P A + hν A = E E + A E + P E + hν E , where ν A and ν E are absorbed and emitted photon frequencies, respectively.…”

“…However, we recently discovered an above-excitation emission, [ 19 , 20 ] hereafter named supracence; when a yellow-green laser excites rhodamine B, higher-frequency green light radiates strongly ( Figure 2 B). Supracence is independent of temperature; thus, it is a linear process or requires only a single step of photoexcitation based on previous data [ 19 , 20 ] and work reported here ( Figure 2 C). This is exciting because, for the first time, the molecules donate their internal energy to the emitted photons, thus emitting higher-energy photons.…”

Azo Pigments Make Raman Spectral Multiplexing More Sensitive

“…Typical tags such as organic dyes often emit broad spectra, which limit the number of resolvable colors from two to five—a situation known as the “color barrier”. 4 Materials such as quantum dots and lanthanide nanocrystals were developed to resolve this barrier by leveraging their intrinsic narrower line widths or creating external information code dimensions, 5 but new complications have emerged. For instance, their relatively bulky size may limit the accessibility of particles to the biomarkers of interest and even alter the biological activities of an object.…”

“…Even though this method has successfully been used in exploring structure–function relationships in cells and tissues, it is challenging to analyze many species with high selectivity and sensitivity under biological conditions. Typical tags such as organic dyes often emit broad spectra, which limit the number of resolvable colors from two to fivea situation known as the “color barrier” . Materials such as quantum dots and lanthanide nanocrystals were developed to resolve this barrier by leveraging their intrinsic narrower line widths or creating external information code dimensions, but new complications have emerged.…”