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  1. Strong coupling between light and mechanical strain forms the foundation for next-generation optical micro- and nano-electromechanical systems. Such optomechanical responses in two-dimensional materials present novel types of functionalities arising from the weak van der Waals bond between atomic layers. Here, by using structure-sensitive megaelectronvolt ultrafast electron diffraction, we report the experimental observation of optically driven ultrafast in-plane strain in the layered group IV monochalcogenide germanium sulfide (GeS). Surprisingly, the photoinduced structural deformation exhibits strain amplitudes of order 0.1% with a 10 ps fast response time and a significant in-plane anisotropy between zigzag and armchair crystallographic directions. Rather than arising due to heating, experimental and theoretical investigations suggest deformation potentials caused by electronic density redistribution and converse piezoelectric effects generated by photoinduced electric fields are the dominant contributors to the observed dynamic anisotropic strains. Our observations define new avenues for ultrafast optomechanical control and strain engineering within functional devices.
    Free, publicly-accessible full text available March 10, 2024
  2. Abstract

    A double-edged sword in two-dimensional material science and technology is optically forbidden dark exciton. On the one hand, it is fascinating for condensed matter physics, quantum information processing, and optoelectronics due to its long lifetime. On the other hand, it is notorious for being optically inaccessible from both excitation and detection standpoints. Here, we provide an efficient and low-loss solution to the dilemma by reintroducing photonics bound states in the continuum (BICs) to manipulate dark excitons in the momentum space. In a monolayer tungsten diselenide under normal incidence, we demonstrated a giant enhancement (~1400) for dark excitons enabled by transverse magnetic BICs with intrinsic out-of-plane electric fields. By further employing widely tunable Friedrich-Wintgen BICs, we demonstrated highly directional emission from the dark excitons with a divergence angle of merely 7°. We found that the directional emission is coherent at room temperature, unambiguously shown in polarization analyses and interference measurements. Therefore, the BICs reintroduced as a momentum-space photonic environment could be an intriguing platform to reshape and redefine light-matter interactions in nearby quantum materials, such as low-dimensional materials, otherwise challenging or even impossible to achieve.

  3. Free, publicly-accessible full text available May 25, 2023
  4. Free, publicly-accessible full text available June 1, 2023
  5. Abstract

    Nonlinear light–matter interaction, as the core of ultrafast optics, bulk photovoltaics, nonlinear optical sensing and imaging, and efficient generation of entangled photons, has been traditionally studied by first-principles theoretical methods with the sum-over-states approach. However, this indirect method often suffers from the divergence at band degeneracy and optical zeros as well as convergence issues and high computation costs when summing over the states. Here, using shift vector and shift current conductivity tensor as an example, we present a gauge-invariant generalized approach for efficient and direct calculations of nonlinear optical responses by representing interband Berry curvature, quantum metric, and shift vector in a generalized Wilson loop. This generalized Wilson loop method avoids the above cumbersome challenges and allows for easy implementation and efficient calculations. More importantly, the Wilson loop representation provides a succinct geometric interpretation of nonlinear optical processes and responses based on quantum geometric tensors and quantum geometric potentials and can be readily applied to studying other excited-state responses.

  6. Free, publicly-accessible full text available June 8, 2023
  7. The metal-to-insulator transition of VO 2 underpins applications in thermochromics, neuromorphic computing, and infrared vision. Ge alloying is shown to elevate the transition temperature by promoting V–V dimerization, thereby expanding the stability of the monoclinic phase to higher temperatures. By suppressing the propensity for oxygen vacancy formation, Ge alloying renders the hysteresis of the transition exquisitely sensitive to oxygen stoichiometry.
    Free, publicly-accessible full text available June 8, 2023