Diagonal Slice Four-Wave Mixing: Natural Separation of Coherent Broadening Mechanisms

We present an ultrafast coherent spectroscopy data acquisition scheme that samples slices of the time domain used in multidimensional coherent spectroscopy to achieve faster data collection than full spectra. We derive analytical expressions for resonance lineshapes using this technique that completely separate homogeneous and inhomogeneous broadening contributions into separate projected lineshapes for arbitrary inhomogeneous broadening. These lineshape expressions are also valid for slices taken from full multidimensional spectra and allow direct measurement of the parameters contributing to the lineshapes in those spectra as well as our own

Hidden Silicon-Vacancy Centers in Diamond

We characterize a high-density sample of negatively charged silicon-vacancy (SiV$^-$) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of \ce{SiV^-} centers that is not typically observed in photoluminescence, and which exhibits significant spectral inhomogeneity and extended electronic $T_2$ times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices

Highly Anisotropic Excitons and Multiple Phonon Bound States in a Van der Waals Antiferromagnetic Insulator

Two-dimensional semiconducting systems, such as quantum wells and transition metal dichalcogenides, are the foundations to investigate low dimensional light-matter interactions. To date, the study of elementary photoexcitation, namely the exciton, in 2D semiconductors with intrinsic magnetic order remains a challenge due to the lack of suitable material platforms. Here, we report an observation of excitons coupled to zigzag antiferromagnetic order in the layered antiferromagnetic insulator NiPS3 using both photoluminescence (PL) and optical reflection spectroscopy. The exciton exhibits a linewidth as narrow as ~350 ueV with near unity linear polarization in the PL spectrum. As the thicknesses of samples is reduced from five layers to bilayers, the PL intensity is drastically suppressed and eventually vanishes in monolayers, consistent with the calculated bandgap being highly indirect for both bilayer and monolayer. We observed strong linear dichroism (LD) over a broad spectra range, which shares the same optical anisotropy axis, being locked to the zigzag direction, as the exciton PL. Both LD and the degree of linear polarization in the exciton PL decrease as the temperature increases and become negligible above the Neel temperature. These observations suggest both optical quantities are probes of the symmetry breaking magnetic order parameter. In addition, a sharp resonance in the LD spectrum is observed with an energy near the exciton PL. There exist over ten exciton-A1g phonon bound states on its high energy side, which likely result from the strong modulation of the ligand-to-metal charge transfer energy by strong electron-lattice interactions. Our work establishes NiPS3 as a new 2D platform for exploring magneto-exciton physics with strong correlations, as well as a building block for 2D heterostructures for engineering physical phenomena with time reversal symmetry breaking.Comment: to be appear in Nature Nanotechnolog

Absolute Phase Calibration in Phase-modulated Multidimensional Coherent Spectroscopy

Establishing the correct phase in multidimensional coherent spectroscopy (MDCS) experiments is critical because the interpretation of quantum pathways is based on the phase of their associated spectral features but is not trivial because the phase introduced by experimental conditions can contaminate the signal. Most phase-modulated MDCS (PM-MDCS) experiments study molecular systems for which the spectra can be phased to produce absorptive lineshapes, but this assumption of absorptive lineshapes can break down in more complicated systems. We present a robust technique for correcting the phase in PM-MDCS experiments and demonstrate accurate spectrum phasing for an anharmonic system

Diagonal Slice Four-wave Mixing: Natural Separation of Coherent Broadening Mechanisms

We present an ultrafast coherent spectroscopy data acquisition scheme that samples slices of the time domain used in multidimensional coherent spectroscopy to achieve faster data collection than full spectra. We derive analytical expressions for resonance lineshapes using this technique that completely separate homogeneous and inhomogeneous broadening contributions into separate projected lineshapes for arbitrary inhomogeneous broadening. These lineshape expressions are also valid for slices taken from full multidimensional spectra and allow direct measurement of the parameters contributing to the lineshapes in those spectra as well as our own

Diagonal Slice Four-Wave Mixing: Natural Separation of Coherent Broadening Mechanisms

We present an ultrafast coherent spectroscopy data acquisition scheme that samples slices of the time domain used in multidimensional coherent spectroscopy to achieve faster data collection than full spectra. We derive analytical expressions for resonance lineshapes using this technique that completely separate homogeneous and inhomogeneous broadening contributions into separate projected lineshapes for arbitrary inhomogeneous broadening. These lineshape expressions are also valid for slices taken from full multidimensional spectra and allow direct measurement of the parameters contributing to the lineshapes in those spectra as well as our own

Electrical, optical, and magnetic properties of amorphous yttrium iron oxide thin films and consequences for non-local resistance measurements

We present magnetic characterization, charge resistivity, and optical photoluminescence measurements on amorphous yttrium iron oxide thin films (a-Y-Fe-O), with supporting comparisons to amorphous germanium (a-Ge) films. We measured magnetic properties with both SQUID magnetometry and polarized neutron reflectometry. These results not only confirm that a-Y-Fe-O is a disordered magnetic material with strong predominantly antiferromagnetic exchange interactions and a high degree of frustration, but also that it is best understood electrically as a disordered semiconductor. As with amorphous germanium, a-Y-Fe-O obeys expectations for variable-range hopping through localized electron states over a wide range of temperature. We also clarify the consequences of charge transport through such a semiconducting medium for non-local voltage measurements intended to probe spin transport in nominally insulating magnetic materials. We further compare non-local resistance measurements made with "quasi-dc" automated current reversal to ac measurements made with a lock-in amplifier. These show that the "quasi-dc" measurement has an effective ac current excitation with frequency up to approximately 22 Hz, and that this effective ac excitation can cause artifacts in these measurements including incorrect sign of the non-local resistance. This comprehensive investigation of non-local resistance measurements in a-Y-Fe-O shows no evidence of spin transport on micrometer length scales, which is contrary to our original work, and in line with more recent investigations by other groups.We acknowledge M. Natale, R. K. Bennet, and D. J. Wesenberg for helpful discussions, assistance in the lab, and contributions to early experiments, and Tao Liu for sample preparation. We gratefully acknowledge support from the NSF (Nos. DMR-1709646 and DMR-2004646). Work at CSU was supported by the U.S. National Science Foundation (Nos. ECCS-1915849 and DMR-2002980). Contributions by G.D. to this research were supported by an appointment to the Intelligence Community Postdoctoral Research Fellowship Program at University of Washington and administered by Oak Ridge Institute for Science and Education through an interagency agreement between the U.S. Department of Energy and the Office of the Director of National Intelligence.https://pubs.aip.org/aip/jap/article/133/22/223901/289528