Resonance enhancement of two-photon absorption of phthalocyanines for 3D optical storage in the presence of hot-band absorption

Makarov, Nikolay S.; Drobizhev, Mikhail; Rebane, Aleksander; Peone, Desiree; Wolleb, Heinz; Spahni, Heinz; Макарова, Е. А.; Luk’yanets, E. A.

doi:10.1117/12.696970

Cited by 5 publications

(6 citation statements)

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“…Although a transition of this type is rather uncommon in C2PEF experiments, there are several reports of similar behavior indicating the presence of the HBA process. [23][24][25][26][27][28] As was suggested by Drobizhev et al 25 the collected fluorescence signal, F (in cnt/s), in this case can be written as a sum of two terms, one describing the excitation via HBA and the other via C2PA,…”

Section: Resultsmentioning

confidence: 99%

“…HBA has been shown to play a crucial role in C2PA measurements, [23][24][25][26][27][28] but has not been discussed in the E2PA literature. The importance of including HBA in the analysis of C2PA data has been detailed in a study by Drobizhev et al, 25 where C2PA and HBA were simultaneously observed in a series of meso-tetra-alkynyl-porphyrins.…”

Section: Introductionmentioning

confidence: 99%

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Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Mikhaylov¹,

Wilson²,

Parzuchowski³

et al. 2021

Preprint

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It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 10 orders of magnitude lower photon flux than its classical counterpart.However, there is a significant controversy regarding the magnitude of this quantum enhancement in excitation efficiency. We investigated the fluorescence signals from Rhodamine 6G and LDS798 excited with a CW laser or an entangled photon pair source at ≈1060 nm. We observed a signal that originates from hot-band absorption (HBA), which is one-photon absorption from thermally-populated vibrational levels of the ground electronic state. This mechanism, which has not been previously discussed in the context of E2PA, produces a signal with a linear power dependence, as would be expected for entangled two-photon excited fluorescence (E2PEF). For the typical conditions under which E2PEF measurements are performed, contributions from the HBA process could lead to a several orders-of-magnitude overestimate of the quantum advantage for excitation efficiency.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Mikhaylov¹,

Wilson²,

Parzuchowski³

et al. 2021

Preprint

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“…Overall, the data show a transition from a quadratic (i.e., C2PA) to a linear (i.e., 1PA) excitation regime. Although a transition of this type is rather uncommon in C2PEF experiments, there are several reports of similar behavior indicating the presence of the HBA process. − As suggested by Drobizhev et al, the collected fluorescence signal, F (in cnt/s), can be written as a sum of two terms, one describing the excitation via HBA and the other via C2PA where N is the number of molecules in the excitation volume, K is the overall fluorescence collection efficiency, ϕ is the excitation photon flux, and σ HBA is the HBA cross section. The σ HBA is a function of the excitation frequency ν and sample temperature T (see the Supporting Information for details).…”

mentioning

confidence: 93%

“…HBA has been shown to play a crucial role in C2PA measurements − but has not been discussed in the E2PA literature. The importance of including HBA in the analysis of C2PA data has been detailed in a study by Drobizhev et al, where C2PA and HBA were simultaneously observed in a series of meso-tetraalkynylporphyrins.…”

mentioning

confidence: 99%

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Mikhaylov

Wilson

Parzuchowski

et al. 2022

J. Phys. Chem. Lett.

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It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 1010 lower photon flux than its classical counterpart, therefore enabling ultralow-power two-photon fluorescence microscopy. However, there is a significant controversy regarding the magnitude of this quantum enhancement in excitation efficiency. We investigated the fluorescence signals from Rhodamine 6G and LDS798 excited with a CW laser or an entangled photon pair source at ∼1060 nm. We observed a signal that originates from hot-band absorption (HBA), which is one-photon absorption from thermally populated vibrational levels of the ground electronic state. This mechanism, which has not been previously discussed in the context of E2PA, produces a signal with a linear power dependence, as would be expected for E2PA. For the typical conditions under which E2PA measurements are performed, contributions from the HBA process could lead to a several orders of magnitude overestimate of the quantum advantage.

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“…Recently, there has been an increased interest in the twophoton absorption (2PA) of porphyrinoids due to their potential applications in optical data storage [1][2][3], optical power limiting [4][5][6][7] and photodynamic therapy [8][9][10]. Even though most commonly available porphyrins have typically relatively small peak 2PA cross sections, σ 2 = 5-25 GM (1 GM = 10 -50 cm 4 s photon -1 ) [11], recent studies showed that their nonlinear absorption in the near-IR range of wavelengths can be significantly increased by introducing various structural modifications.…”

Section: Introductionmentioning

confidence: 99%

Two-photon absorption spectroscopy of corroles

et al. 2009

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We report simultaneous two-photon absorption (2PA) spectra in a series of substituted corroles and related porphyrins in 800-1400 nm laser wavelength range. Compared to the porphyrins, the 2PA spectrum of corroles contains a distinct and relatively high intensity peak, σ 2 = 60-130 GM, close to twice the wavelength of Soret maximum (800-850 nm). The increase of 2PA peak cross section is explained in terms of decreased symmetry of the contracted macro-cycle, and is most likely related to relaxing of the parity selection rules that restrict 2PA in the Soret band for more symmetrical porphyrins. We also observe that the strength of the 2PA peak in Soret region decreases with the electron-withdrawing ability (increasing Hammett constant) of the side substituents, which can be explained by assuming that the corrole core itself possesses electron-accepting ability. The peak 2PA cross sections in the Q-region are much less than in Soretregion, and can be quantitatively described within the two-level approximation taking into account permanent dipole moments in the ground and excited states.

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Resonance enhancement of two-photon absorption of phthalocyanines for 3D optical storage in the presence of hot-band absorption

Cited by 5 publications

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Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Hot-Band Absorption Can Mimic Entangled Two-Photon Absorption

Two-photon absorption spectroscopy of corroles

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