تم التحقق من إثارة أربعة وحدات فونون متوازنة من أنماط مختلفة في الميتابورات النحاسية CuB$_2$O$_4$ عن طريق الانبعاث الشديد المشجع الراماني (ISRS). وتم كشف الفونونات بمراقبة التغيرات في البيريفرنج البصري الخطي باستخدام تقنية الكشف المتوازن (BD). نقارن نتائج تجربة BD-ISRS ببيانات مجموعة من الفونونات الشواردية الرامانية المولودة بشكل طبيعي. نظرا للتوافق الذي تحققناه بين هذين الطريقتين في مدى واسع من ترددات الفونونات من 4 إلى 14 تيراهرتز، يجب أن نتأكد من التناسب الدقيق بين تركيب الفونونات وقواعد الإثارة والكشف المتوقعة. كما يؤثر في هذا التحليل المقارن أيضا الفرق بين الفونونات الغير متوازنة والمتوازنة بشأن مساهمتهم في عملية الانبعاث الراماني. ويسلط الضوء على أهمية نسبة بين تردد وحدة فونون معينة وعرض الطيف الخاص بالطاقة المشجعة والمستشعرة. ونظرا لذلك نظرنا أنه يجب أن نوضح بشكل تحليلي أن مدتي الطاقة المشجعة والمستشعرة التي تستخدم في تجاربنا، التي هي 90 و 50 فولت ثانية على التوالي، تحدد أعلى تردد للوحدات الفونون المثيرة والمحسوسة المتوازنة إلى 12 تيراهرتز، وتحدد أجزاؤها النسبية.
Excitation of four coherent phonon modes of different symmetries has been realized in copper metaborate CuB$_2$O$_4$ via impulsive stimulated Raman scattering (ISRS). Phonons were detected by monitoring changes in the linear optical birefringence using the balanced-detection (BD) technique. We compare the results of BD-ISRS experiment to the polarized spontaneous Raman scattering spectra. We show that the agreement between the two sets of data obtained by these allied techniques in a wide phonon frequencies range of 4-14 THz can be achieved by rigorously taking into account the symmetry of the phonon modes, and the corresponding excitation and detection selection rules. It is also important to account for the difference between incoherent and coherent phonons in terms of their contributions to the Raman scattering process. This comparative analysis highlights the importance of the ratio between the frequency of a particular mode, and the pump and probe spectral widths. We demonstrate analytically that the pump and probe pulse durations of 90 and 50 fs, respectively, used in our experiments, limit the highest frequency of the excited and detected coherent phonon modes to 12 THz, and define their relative amplitudes.
The global optimum for valence population transfer in the NO$_2$ molecule driven by impulsive x-ray stimulated Raman scattering of one-femtosecond x-ray pulses tuned below the Oxygen K-edge is determined with the Multiconfiguration Time-Dependent Hartree-Fock method, a fully-correlated first-principles treatment that allows for the ionization of every electron in the molecule. Final valence state populations computed in the fixed-nuclei, nonrelativistic approximation are reported as a function of central wavelength and intensity. The convergence of the calculations with respect to their adjustable parameters is fully tested. Fixing the 1fs duration but varying the central frequency and intensity of the pulse, without chirp, orientation-averaged maximum population transfer of 0.7% to the valence B$_1$ state is obtained at an intensity of 3.16$times$10$^{17}$ W cm$^{-2}$, with the central frequency substantially 6eV red-detuned from the 2nd order optimum; 2.39% is obtained at one specific orientation. The behavior near the global optimum, below the Oxygen K-edge, is consistent with the mechanism of nonresonant Raman transitions driven by the near-edge fine structure oscillator strength.
Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper reports an inelastic light scattering study of the magnon and phonon spectrum of CoCr$_2$O$_4$ as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature ($T_C sim 94$ K) of CoCr$_2$O$_4$ we observe a $omega sim 16 ,text{cm}^{-1}$ $boldsymbol q=0$ magnon having T$_{1g}$-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T$_{1g}$-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr$_2$O$_4$. The Raman susceptibility of the T$_{1g}$-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr$_2$O$_4$, suggesting that magnetodielectric behavior in CoCr$_2$O$_4$ primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr$_2$O$_4$ with applied pressure decreases the magnetic field-dependence of the T$_{1g}$-symmetry magnon Raman susceptibility in CoCr$_2$O$_4$, suggesting that strain can be used to control the magnetodielectric response in CoCr$_2$O$_4$.
The interaction between ultrashort light pulses and non-absorbing materials is dominated by Impulsive Stimulated Raman Scattering (ISRS). The description of ISRS in the context of pump&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by means of spectrally resolved pump&probe measurements on $alpha$-quartz.
We have calculated the resonant and nonresonant contributions to attosecond impulsive stimulated electronic Raman scattering (SERS) in regions of autoionizing transitions. Comparison with Multiconfiguration Time-Dependent Hartree-Fock (MCTDHF) calculations find that attosecond SERS is dominated by continuum transitions and not autoionizing resonances. These results agree quantitatively with a rate equation that includes second-order Raman and first-and second-order photoionization rates. Such rate models can be extended to larger molecular systems. Our results indicate that attosecond SERS transition probabilities may be understood in terms of two-photon generalized cross sections even in the high-intensity limit for extreme ultraviolet wavelengths.
We have studied the coherent dynamics of G-band phonons in single-walled carbon nanotubes through impulsive stimulated Stokes and anti-Stokes Raman scattering. The probe energy dependence of phonon amplitude as well as preferential occurrence between Stokes and anti-Stokes components in response to chirped-pulse excitation are well explained within our model. The temperature dependence of the observed dephasing rate clearly exhibits a thermally-activated component, with an activation energy that coincides with the frequency of the radial breathing mode (RBM). This fact provides a clear picture for the dephasing of optical phonons by random frequency modulation via interaction with the RBM through anharmonicity.