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Shraddha M. Rao

Publications and source records attributed to Shraddha M. Rao.

4 recordsLinked to original sources

Unraveling the Roles of Shallow, Deep and Auger Trapping in Charge Carrier Recombination in Triple-Cation Perovskites

Understanding charge-carrier recombination in metal halide perovskites is essential for accurately identifying the factors limiting solar cell efficiency, yet it remains challenging due to the interplay of multiple competing processes. Here, we combine time-resolved photoluminescence and excitation dependent photoluminescence quantum yield measurements over a wide range of fluences and repetition rates to investigate recombination dynamics in triple-cation perovskite thin films. By jointly analyzing these multidimensional datasets, we develop a unified model that quantitatively reproduces both photoluminescence decays and absolute quantum yields across all excitation conditions. Our results reveal the coexistence of deep and shallow traps, as well as a second-order nonradiative recombination pathway attributed to Auger-assisted trapping. Importantly, this mechanism dominates under one-sun illumination, making it a critical limiting factor for photovoltaic performance. These findings provide a comprehensive framework for understanding recombination in perovskites and highlight the importance of higher-order defect-mediated processes in determining their efficiency.

cond-mat.mtrl-sci↗

Memlumor: a luminescent memory device for photonic neuromorphic computing

Neuromorphic computing promises to transform the current paradigm of traditional computing towards Non-Von Neumann dynamic energy-efficient problem solving. Thus, dynamic memory devices capable of simultaneously performing nonlinear operations (volatile) similar to neurons and also storing information (non-volatile) alike brain synapses are in the great demand. To satisfy these demands, a neuromorphic platform has to possess intrinsic complexity reflected in the built-in diversity of its physical operation mechanisms. Herein, we propose and demonstrate the novel concept of a memlumor - an all-optical device combining memory and luminophore, and being mathematically a full equivalence of the electrically-driven memristor. By utilizing metal halide perovskites as a memlumor material platform, we demonstrate the synergetic coexistence of both volatile and non-volatile memory effects within a broad timescale from ns to days. We elucidate the origin of such complex response to be related to the phenomena of photodoping and photochemistry activated by a tunable light input and explore several possible realizations of memlumor computing. Leveraging on the existence of a history-dependent photoluminescent quantum yield in various material platforms, the memlumor device concept will trigger multiple new research directions in both material science and optoelectronics. We anticipate that the memlumor, as a new optical dynamic computing element, will add a new dimension to existing optical technologies enabling their transition into application in photonic neuromorphic computing.

physics.optics↗

Two-dimensional materials and the coherent control of nonlinear optical interactions

Deeply sub-wavelength two-dimensional films may exhibit extraordinarily strong nonlinear effects. Here we show that 2D films exhibit the remarkable property of a phase-controllable nonlinearity, i.e., the amplitude of the nonlinear polarisation wave in the medium can be controlled via the pump beam phase and determines whether a probe beam will "feel" or not the nonlinearity. This is in stark contrast to bulk nonlinearites where propagation in the medium averages out any such phase dependence. We perform a series of experiments in graphene that highlight some of the consequences of the optical nonlinearity phase-dependence, {such as} the coherent control of nonlinearly diffracted beams, single-pump-beam {induced} phase-conjugation and the demonstration of a nonlinear mirror characterised by negative reflection. The observed phase sensitivity is not specific to graphene but rather is solely a result of the dimensionality and is therefore expected in all 2D materials.

physics.optics↗

Coherent control of light interaction with graphene

We report the experimental observation of all-optical modulation of light in a graphene film. The graphene film is scanned across a standing wave formed by two counter-propagating laser beams in a Sagnac interferometer. Through a coherent absorption process the on-axis transmission is modulated with close to 80% efficiency. Furthermore we observe modulation of the scattered energy by mapping the off-axis scattered optical signal: scattering is minimized at a node of the standing wave pattern and maximized at an antinode. The results highlight the possibility to switch and modulate any given optical interaction with deeply sub-wavelength films.

physics.optics↗