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Nanomaterials

The Asymmetry Observed between the Effects of Photon–Phonon Coupling and Crystal Field on the Fine Structure of Fluorescence and Spontaneous Four-Wave Mixing in Ion-Doped Microcrystals

Huanrong Fan, Zhongtai Zhang, Iqbal Hussain, Qinyue Yang, Muhammad Kashif Majeed, Muhammad Imran, Faizan Raza, Peng Li, Yanpeng Zhang

Published Apr 12, 2024• 4 citations
Publisher

Abstract

In this paper, we explore the asymmetry observed between the effects of photon–phonon coupling (nested-dressing) and a crystal field (CF) on the fine structure of fluorescence (FL) and spontaneous four-wave mixing (SFWM) in Eu3+: BiPO4 and Eu3+: NaYF4. The competition between the CF and the strong photon–phonon dressing leads to dynamic splitting in two directions. The CF leads to static splitting in one direction under weak phonon dressing. The evolution from strong dressing to weak dressing results in spectral asymmetry. This spectral asymmetry includes out-of-phase FL and in-phase SFWM. Further, the large ratio between the dressing Rabi frequency and the de-phase rate leads to strong FL and SFWM asymmetry due to photon–phonon constructive dressing. Moreover, the experimental results suggest the analogy of a spectra asymmetry router with a channel equalization ratio of 96.6%.

DOI
10.3390/nano14080671

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In this paper, we explore the asymmetry observed between the effects of photon–phonon coupling (nested-dressing) and a crystal field (CF) on the fine structure of fluorescence (FL) and spontaneous four-wave mixing (SFWM) in Eu3+: BiPO4 and Eu3+: NaYF4. The competition between the CF and the strong photon–phonon dressing leads to dynamic splitting in two directions. The CF leads to static splitting in one direction under weak phonon dressing. The evolution from strong dressing to weak dressing results in spectral asymmetry. This spectral asymmetry includes out-of-phase FL and in-phase SFWM. Further, the large ratio between the dressing Rabi frequency and the de-phase rate leads to strong FL and SFWM asymmetry due to photon–phonon constructive dressing. Moreover, the experimental results suggest the analogy of a spectra asymmetry router with a channel equalization ratio of 96.6%.
We report the multi-Fano interference obtained through the simultaneous acquisition of bright and dark states in different phase transitions of Eu3+: BiPO4 (7:1, 6:1, 1:1, and 0.5:1) and Eu3+: NaYF4 (1:1/4) crystals. We employ multi-dressed spontaneous four-wave mixing and multi-dressed fluorescence (multi-order) to optimize the strong photon-phonon nested dressing effect resulting in more obvious multi-Fano interference. Firstly, the multi-Fano is produced through interference in continuous and multi-bound states. Secondly, five multi-Fano dips originate from nested five dressings (one photon and four phonons) under symmetrical splitting of 7F1 energy level. We depict that the pure H-phase (0.5:1) sample exhibits the strongest photon-phonon dressed effect (five Fano dips). Further, we investigate high-order non-Hermitian exceptional points in multi-Fano interference by adjusting the ratio of Rabi-frequency to de-phase rate through nested photon and phonon dressing. Our experimental results are validated by theoretical simulations, which may be applied to designing optoelectronic devices such as non-Hermitian multi-Fano interferences (multi-channel) router.
We report super broad non-Hermitian line shape from out-of-phase and in-phase photon-phonon dressing (quantization) in Eu3+: NaYF4 and Eu3+: BiPO4 nanocrystals. The line shape is controlled by changing time gate position, time gate width, power, temperature, sample, photomultiplier tubes, and laser. We observed that the fluorescence (FL) line-shape contrasts are 69.23% for Eu3+: BiPO4 and 43.75% for Eu3+: NaYF4, owing to the stronger out-of-phase photon-phonon dressing (destructive quantization). Moreover, we observed that the spontaneous four-wave mixing (SFWM) line shape was approximately three times wider at 300 K than at 77 K for the [(12:1)-phase] Eu3+: NaYF4 due to more high-frequency in-phase phonon dressing (strong constructive quantization). Furthermore, we showed that the noise line-shape width remains unchanged for Eu3+: BiPO4 (16 nm) and Eu3+: NaYF4 (12 nm) due to out-of-phase and in-phase photon-phonon dressing balance. Such results have potential applications in multi-channel band stop filter.
We investigate the effect of single dressing and double dressing on fourth-order fluorescence (FL) and spontaneous four-wave mixing. The single dressing effect changes to a double dressing effect as we change the detuning (power) of the input beam from off-resonant (low power) to resonant point (high power). We also demonstrate the spectral and temporal nature of fourth-order FL and its Autler–Townes splitting caused by the competition of the phonon effect (at different temperatures) with a single and double dressed state in Pr3+:Y2SiO5 crystal. To further explore the competition between the phonon and dressing effects, we investigated intensity-noise correlation of spontaneous parametric four-wave mixing at 110 K. Our results demonstrate the dependency of YSO crystal on temperature, detuning, and power, which can be controlled by the competition between a phonon with single and double dressing.
crystal. Such atomic coherence spectral interaction evolves from out-of-phase fluorescence to in-phase spontaneous four-wave mixing (SFWM) by changing the time gate. The dressing dip switch and three dressing dips of SFWM result from the strong photon-phonon destructive cross- and self-interaction for the hexagonal phase, respectively. More phonon dressing results in the destructive interaction, while less phonon dressing results in the constructive interaction of the atomic coherences. The experimental measurements of the photon-phonon interaction agree with the theoretical simulations. Based on our results, we proposed a model for an optical transistor (as an amplifier and switch).
Abstract Laser interaction with doped crystals exhibiting photon–photon and photon–phonon coupling has been focused on recently. In pretext, here we report the spectral and temporal profile interaction of two lasers excitation through various phases of Eu3+: BiPO4 crystals. We reveal that spectral-temporal profile interaction of hybrid signals (coexisting fluorescence and spontaneous four-wave mixing) are dressed by nested and cascade processes of two-photons (two-phonon). Such interaction comes from thermal phonon constructive and phase transition phonon destructive dressing. The spectral and temporal (profile) interactions are interrelated and reduced by about 2-times due to two-photon nested dressing in contrast to the interaction through the sum of each laser excitation. In contrast to a single laser, spectral (Fano)-dip interaction reduces by 2-times due to two-photon destructive dressing coupling. Moreover, thermal phonon dressing at 300 K exhibits 3-times more extensive temporal interaction than that at 77 K. The phase transition phonon dressing for a half hexagonal and half low-temperature monoclinic phase is about 1.5-times longer than that of the pure hexagonal phase of Eu3+: BiPO4. These results may help to understand the spectral-temporal relationship in the fields of nonlinear and quantum optics.
We report photon-phonon dressing quantization dependency on polarization. Destructive dressing polarization quantization is exhibited in fluorescence (FL) for narrowband signals, while constructive dominant dressing quantization is exhibited in fluorescence (FL) for broadband signals due to phase perturbation. Furthermore, constructive polarization quantization results due to coexistence of generation and dressing effects in strong and competitive Rabi frequency. Low power also contributes to more dressing polarization quantization, the same as in the FL region (large de-phase rate). Furthermore, linear and circular dressing quantization with polarization quantization shows inverse and direct relationships in the FL and spontaneous four-wave-mixing (SFWM) regions, respectively. Such investigations have potential in alignment of crystal field (CF) redistribution by polarization quantization at the input.