Brandon Yalin

“Hidden” phases, generated using ultrafast laser pulses (few hundred femtoseconds), with distinct properties than at the thermodynamic equilibrium, are appealing for technologies, as they can be long-lived, with a lifetime of hours or weeks, and reversible with temperature sweeping or extra pulses. In this regard, La 2 / 3 Ca 1 / 3 MnO 3 (LCMO) stands out due to its tunability through epitaxial strain, which can drive the bulk ferromagnetic metal into an antiferromagnetic insulator (AFI), and its susceptibility to photoinduced transitions. Indeed, AFI LCMO displays a long-lived photoinduced transition into a putative hidden phase whose exact nature and excitations are still largely unknown. Here, we combine ultrafast photoexcitation in the near infrared with transport, x-ray absorption, and resonant inelastic x-ray scattering (RIXS) to investigate the excitations (polarons, phonons, and orbital) of the photoexcited phase of LCMO and contrast them with the thermodynamic phases achieved through strain and temperature. In the thermodynamic regime, we establish the correlation between polarons and transport placing them in the “strong coupling” regime of the Holstein model. Upon photoexcitation of LCMO-AFI, we uncover a long-lived phase characterized by the softening of the polaron excitations, the partial suppression of the Jahn-Teller distortion, and nearly unchanged phonons, showing the emergence of a photoexcited state absent in the equilibrium phase diagram. Finally, by varying temperature, epitaxial strain, and photoexcitation fluence, we construct a polaron phase diagram and identify the key spectroscopic signatures of each phase. Our laser-RIXS approach establishes a versatile platform for exploring photoinduced hidden phases in quantum materials in nonstroboscopic conditions.

Energy transfer (ET) from nanocrystals (NCs) has shown potential to enhance the optoelectronic performance of ultrathin semiconductor devices such as ultrathin Si solar cells, but the experimental identification of optimal device geometries for maximizing the performance enhancement is highly challenging due to a large parameter space. Here, we have demonstrated a general theoretical framework combining transfer matrix method (TMM) simulations and energy transfer (ET) calculations to reveal critical device design guidelines for developing an efficient, NC-based ET sensitization of ultrathin Si solar cells, which are otherwise infeasible to identify experimentally. The results uncover that the ET-driven NC sensitization is highly effective in enhancing the short circuit current (J_SC) in sub-100 nm-thick Si layers, where, for example, the ET contribution can account for over 60% of the maximum achievable J_SC in 10 nm-thick ultrathin Si. The study also reveals the limitation of the ET approach, which becomes ineffective for Si active layers thicker than 5 μm, being dominated by conventional optical coupling. The demonstrated simulation approach not only enables the development of efficient ultrathin Si solar cells but also should be applicable to precisely assessing and analyzing diverse experimental device geometries and configurations for developing new efficient ET-based ultrathin semiconductor optoelectronic devices.