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Register a new userNonreciprocal second harmonic generation in a magnetoelectric material
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Nonreciprocal devices that allow the light propagation in only one direction are indispensable in photonic circuits and emerging quantum technologies. Contemporary optical isolators and circulators, however, require large size or strong magnetic fields because of the general weakness of magnetic light-matter interactions, which hinders their integration into photonic circuits. Aiming at stronger magneto-optical couplings, a promising approach is to utilize nonlinear optical processes. Here, we demonstrate nonreciprocal magnetoelectric second harmonic generation (SHG) in CuB2O4. SHG transmission changes by almost 100% in a magnetic-field reversal of just 10 mT. The observed nonreciprocity results from an interference between the magnetic-dipole- and electric-dipole-type SHG. Even though the former is usually notoriously smaller than the latter, it is found that a resonantly enhanced magnetic-dipole-transition has a comparable amplitude as non-resonant electric-dipole-transition, leading to the near-perfect nonreciprocity. This mechanism could form one of the fundamental bases of nonreciprocity in multiferroics, which is transferable to a plethora of magnetoelectric systems to realize future nonreciprocal and nonlinear-optical devices.
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Giant second-harmonic generation (SHG) in the terahertz (THz) frequency range is observed in a thin film of an s-wave superconductor NbN, where the time-reversal ($mathcal{T}$-) and space-inversion ($mathcal{P}$-) symmetries are simultaneously broken by supercurrent injection. We demonstrate that the phase of the second-harmonic (SH) signal flips when the direction of supercurrent is inverted, i.e., the signal is ascribed to the nonreciprocal response that occurs under broken $mathcal{P}$- and $mathcal{T}$-symmetries. The temperature dependence of the SH signal exhibits a sharp resonance, which is accounted for by the vortex motion driven by the THz electric field in an anharmonic pinning potential. The maximum conversion ratio $eta_{mathrm{SHG}}$ reaches $approx10^{-2}$ in a thin film NbN with the thickness of 25 nm after the field cooling with a very small magnetic field of $approx1$ Oe, for a relatively weak incident THz electric field of 2.8 kV/cm at 0.48 THz.
Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations.
The notion of spontaneous symmetry breaking has been used to describe phase transitions in a variety of physical systems. In crystalline solids, the breaking of certain symmetries, such as mirror symmetry, is difficult to detect unambiguously. Using 1$T$-TaS$_2$, we demonstrate here that rotational-anisotropy second harmonic generation (RA-SHG) is not only a sensitive technique for the detection of broken mirror symmetry, but also that it can differentiate between mirror symmetry-broken structures of opposite planar chirality. We also show that our analysis is applicable to a wide class of different materials with mirror symmetry-breaking transitions. Lastly, we find evidence for bulk mirror symmetry-breaking in the incommensurate charge density wave phase of 1$T$-TaS$_2$. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role.
Strong second-harmonic generation has recently been experimentally observed from metamaterials consisting of periodic arrays of metal split ring resonators with an effective negative magnetic permeability [Science, 313, 502 (2006)]. To explore the underlying physical mechanism, a classical model derived from microscopic theory is employed here. The quasi-free electrons inside the metal are approximated as a classical Coulomb-interacting electron gas, and their motion under the excitation of an external electromagnetic field is described by the cold-plasma wave equations. Through numerical simulations, it is demonstrated that the microscopic theory includes the dominant physical mechanisms bothqualitatively and quantitatively.
Second harmonic generation (SHG) spectroscopy ubiquitously enables the investigation of surface chemistry, interfacial chemistry as well as symmetry properties in solids. Polarization-resolved SHG spectroscopy in the visible to infrared regime is regularly used to investigate electronic and magnetic orders through their angular anisotropies within the crystal structure. However, the increasing complexity of novel materials and emerging phenomena hamper the interpretation of experiments solely based on the investigation of hybridized valence states. Here, polarization-resolved SHG in the extreme ultraviolet (XUV-SHG) is demonstrated for the first time, enabling element-resolved angular anisotropy investigations. In non-centrosymmetric LiNbO$_3$, elemental contributions by lithium and niobium are clearly distinguished by energy dependent XUV-SHG measurements. This element-resolved and symmetry-sensitive experiment suggests that the displacement of Li ions in LiNbO$_3$, which is known to lead to ferroelectricity, is accompanied by distortions to the Nb ion environment that breaks the inversion symmetry of the NbO$_{6}$ octahedron as well. Our simulations show that the measured second harmonic spectrum is consistent with Li ion displacements from the centrosymmetric position by $sim$0.5 Angstrom while the Nb-O bonds are elongated/contracted by displacements of the O atoms by $sim$0.1 Angstrom. In addition, the polarization-resolved measurement of XUV-SHG shows excellent agreement with numerical predictions based on dipole-induced SHG commonly used in the optical wavelengths. This constitutes the first verification of the dipole-based SHG model in the XUV regime. The findings of this work pave the way for future angle and time-resolved XUV-SHG studies with elemental specificity in condensed matter systems.
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