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Burak Guzelturk

Publications and source records attributed to Burak Guzelturk.

12 recordsLinked to original sources

Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics↗

Tracking thermal transport in colloidal quantum dot films using in-situ time-resolved X-ray diffraction

Colloidal quantum dots (QDs) and their thin-films are increasingly used in electronic and photonic devices replacing traditional bulk semiconductors. However, thermal properties of the QDs are comparatively underexplored relative to device development efforts. This study shows the use of time-resolved X-ray diffraction as a contact-free method to probe the thermal response of QDs in device-like environments, providing in-situ insights for future thermal management strategies. Through the extraction of Debye-Waller Factors on a sub-nanosecond timescale, we use time-resolved X-ray diffraction to directly capture the heating and cooling of core/shell CdSe/CdS QDs following pulsed optical excitation. In a QD thin-film that actively provides optical gain, the thermal conductivity is found to be as low as 0.55 $\mathrm{W\,m^{-1}\,K^{-1}}$, because of the poor heat flow within close-packed QD solids. For QDs dispersed in liquids, interfacial thermal conductance is found to dominate the thermal relaxation with a conductance on the order of 15 $\mathrm{MW\,m^{-2}\,K^{-1}}$.

cond-mat.mes-hall↗

Photoinduced metastable cation disorder in metal halide double perovskites

Lead-free perovskites have emerged as environmentally benign alternatives to lead-halide counterparts for optoelectronics. Among them, the double perovskite Cs2AgInCl6 family exhibits remarkable white-light emission with proper composition engineering, enabled by strong electron-phonon coupling and the formation of self-trapped excitons (STEs). Despite these advantages, the fundamental photo- and structural dynamics governing their excited-state behavior remain poorly understood. Here, we report a long-lived metastable phase in the Cs2AgInCl6 double perovskite family and unravel this process and the concomitant electronic and structural evolution using a suite of tools including transient optical spectroscopy, time-resolved X-ray diffraction (TR-XRD) and X-ray absorption (TR-XAS). We show that the photoinduced, transient metastable phase is associated with B-site (Ag-In) disorder, which induces a dramatically reduced optical bandgap. Supported by TR-XRD and first-principles calculations, the Ag-In disorder drives the formation of Ag-rich and In-rich domains with millisecond lifetimes, with lifetimes increasing at lower temperatures. TR-XAS further reveals that photogenerated STEs oxidize Ag+ to Ag2+, facilitating this highly temporally asymmetric order-disorder transition. Our findings demonstrate a new mechanism, mediated by hole-localized STE formation, that enables prolongation of transient light-induced states to the multi-millisecond regime in double perovskites, opening possibilities to harvesting the functional properties of metastable phases of these materials.

cond-mat.mtrl-sci↗

Ultrafast light-induced formation of a metastable hidden state in bismuth vanadate

Bismuth vanadate (BiVO$_4$) is a key photocatalyst for solar fuel applications, yet fundamental questions remain regarding the nature of photogenerated polaronic states and the lattice dynamics that govern its light-to-chemical pathways. Here, we use femtosecond optical pump-X-ray probe measurements to track the photoinduced electronic and structural dynamics in BiVO$_4$ across multiple length and time scales. Transient X-ray absorption spectroscopy captures sub-picosecond electron localization within VO$_4$ tetrahedra, consistent with small polaron formation, whereas time-resolved X-ray diffraction reveals a slower, multi-picosecond lattice reorganization into a hidden photoexcited state that is structurally distinct from both the monoclinic ground state and the high-temperature tetragonal phase. Supported by density functional theory, we show that hole-lattice interactions dynamically reduce the ground state monoclinic distortion, stabilizing the hidden state. Our results demonstrate that electron- and hole-lattice coupling jointly shape the excited state landscape, with implications for carrier transport, interfacial energetics, and light-to-chemical energy conversion pathways.

cond-mat.mtrl-sci↗

Ultrafast symmetry control in photoexcited quantum dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, we unveil reversible symmetry changes in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, we reveal that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties as shown by transient optical measurements. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

cond-mat.mes-hall↗

Optical Control of Adaptive Nanoscale Domain Networks

Adaptive networks can sense and adjust to dynamic environments to optimize their performance. Understanding their nanoscale responses to external stimuli is essential for applications in nanodevices and neuromorphic computing. However, it is challenging to image such responses on the nanoscale with crystallographic sensitivity. Here, the evolution of nanodomain networks in (PbTiO3)n/(SrTiO3)n superlattices was directly visualized in real space as the system adapts to ultrafast repetitive optical excitations that emulate controlled neural inputs. The adaptive response allows the system to explore a wealth of metastable states that were previously inaccessible. Their reconfiguration and competition were quantitatively measured by scanning x-ray nanodiffraction as a function of the number of applied pulses, in which crystallographic characteristics were quantitatively assessed by assorted diffraction patterns using unsupervised machine-learning methods. The corresponding domain boundaries and their connectivity were drastically altered by light, holding promise for light-programmable nanocircuits in analogy to neuroplasticity. Phase-field simulations elucidate that the reconfiguration of the domain networks is a result of the interplay between photocarriers and transient lattice temperature. The demonstrated optical control scheme and the uncovered nanoscopic insights open opportunities for remote control of adaptive nanoscale domain networks.

cond-mat.mes-hall↗

Hidden correlations in stochastic photoinduced dynamics of a solid-state electrolyte

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and offering a microscopic view of complex dynamics at the molecular level. The photo response following a laser pulse is, in general, non-identical between multiple exposures due to spatiotemporal fluctuations in a material or the stochastic nature of dynamical pathways. However, most ultrafast experiments using a stroboscopic pump-probe scheme struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing seemingly random deviations from the averaged shot-to-shot response. Leveraging the stability and high photon-flux of time-resolved X-ray micro-diffraction at a synchrotron, we developed a method to quantitatively characterize the shot-to-shot variation of the photoinduced dynamics in a solid-state electrolyte. By analyzing temporal evolutions of the lattice parameter of a single grain in a powder ensemble, we found that the sample responses after different shots contain random fluctuations that are, however, not independent. Instead, there is a correlation between the nonequilibrium lattice trajectories following adjacent laser shots with a characteristic "correlation length" of approximately 1,500 shots, which represents an energy barrier of 0.38~eV for switching the photoinduced pathway, a value interestingly commensurate with the activation energy of lithium ion diffusion. Not only does our nonequilibrium noise correlation spectroscopy provide a new strategy for studying fluctuations that are central to phase transitions in both condensed matter and molecular systems, it also paves the way for discovering hidden correlations and novel metastable states buried in oft-presumed random, uncorrelated fluctuating dynamics.

cond-mat.mtrl-sci↗

Phonon-Mediated Attractive Interactions between Excitons in Lead-Halide-Perovskites

Understanding the origin of electron-phonon coupling in lead-halide perovskites (LHP) is key to interpreting and leveraging their optical and electronic properties. Here we perform femtosecond-resolved, optical-pump, electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in LHP nanocrystals. Photoexcitation is found to drive a reduction in lead-halide octahedra tilts and distortions in the lattice, a result of deformation potential coupling to low energy optical phonons. Our results indicate particularly strong coupling in FAPbBr3, and far weaker coupling in CsPbBr3, highlighting differences in the dominant machanisms governing electron-phonon coupling in LHPs. We attribute the enhanced coupling in FAPbBr3 to its disordered crystal structure, which persists down to cryogenic temperatures. We find the reorganizations induced by each exciton in a multiexcitonic state constructively interfere, giving rise to a coupling strength which scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in LHPs.

cond-mat.mtrl-sci↗

Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in nanocrystals are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in semiconductor nanocrystals. Investigation of the excitation energy dependence shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap result in transient lattice heating that occurs on a much longer 200 ps timescale, governed by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

cond-mat.mes-hall↗

Orientation-Controlled Construction of Superstructures of Atomically-Flat Nanocrystals: Pushing the Limits of Ultra-Thin Colloidal Gain Media

We propose and demonstrate a method for the construction of highly uniform, multilayered, orientation-controlled superstructures of CdSe/CdZnS core/shell colloidal nanoplatelets (NPLs) using bi-phase liquid interface. These atomically-flat nanocrystals are sequentially deposited, all face-down onto a solid substrate, into slabs having monolayer-precise thickness and excellent homogeneity over several tens of cm2 areas. Owing to the near-unity surface coverage and film uniformity of this deposition technique, amplified spontaneous emission (ASE) is observed from an uncharacteristically thin colloidal film having only 6 layers of NPLs, which corresponds to a mere 42 nm thickness. Furthermore, systematic studies of optical gain properties of these NPL superstructures constructed having precise numbers of NPL layers tuned from 6 to 15 revealed the reduction in the gain threshold with the increasing number of NPL monolayers, along with a continuous spectral shift in the position of the ASE peak (by ~18 nm). These observations can be well explained by the variation of the optical field confinement factor with the NPL waveguide thickness and propagation wavelength. This work demonstrates the possibility of fabricating thickness-tunable, large-area three-dimensional superstructures made of NPL building blocks, which can be additively constructed one monolayer at a time. The proposed technique can also be extended to build hybrid NPL films of mixed orientations and allow for precise large-area device engineering.

physics.app-ph↗

Sub-single exciton optical gain threshold in colloidal semiconductor quantum wells with gradient alloy shelling

Colloidal semiconductor quantum wells have emerged as a promising material platform for use in solution-processable light-generation including colloidal lasers. However, application relying on their optical gain suffer from a fundamental complication due to multi-excitonic nature of light amplification in common II-VI semiconductor nanocrystals. This undesirably increases the optical gain threshold and shortens the net gain lifetime because of fast nonradiative Auger decay. Here, we demonstrate sub-single exciton level of optical gain threshold in specially engineered CdSe/CdS@CdZnS core/crown@gradient alloyed shell colloidal quantum wells. This sub-single exciton ensemble-averaged gain threshold of Ng = 0.80 (per particle) resulting from impeded Auger recombination along with a large absorption cross-section of quantum wells enables us to observe the amplified spontaneous emission starting at a low pump fluence of 800 nJ cm-2, at least three-folds better than the previously best reported values among all colloidal semiconductor nanocrystals. Moreover, long optical gain lifetimes of 800 ps accompanied with modal gain coefficients of 2,000 cm-1 are achieved. Finally, using these gradient shelled quantum wells, we show a vertical cavity surface-emitting colloidal laser operating at an ultralow lasing threshold of 7.5 micro-joule cm-2. These results represent a significant step towards the realization of solution-processable electrically-driven colloidal lasers.

physics.app-ph↗

Copper-Doped Colloidal Semiconductor Quantum Wells for Luminescent Solar Concentrators

Doping of bulk semiconductors has revealed widespread success in optoelectronic applications. In the past few decades, substantial effort has been engaged for doping at the nanoscale. Recently, doped zero-dimensional quantum dots made of semiconductor nanocrystals have been demonstrated to be promising materials for luminescent solar concentrators (LSCs) as they can be engineered for providing Stokes-shifted tunable emission in the solar spectrum. However, existing doped colloidal quantum dots suffer from moderately low quantum efficiency and intrinsically small absorption cross-section, which together fundamentally limit their effective usage. Here, we show the first account of copper doping into two-dimensional atomically flat CdSe colloidal quantum wells. Copper doping via post-synthesis partial cation exchange into 3-5 monolayers of CdSe and CdSe/CdS core-shell colloidal quantum wells (CQWs) enables Stokes-shifted, tunable dopant induced highly efficient photoluminescence emission having high quantum efficiencies (>43%), accompanied by an order of magnitude higher absorption cross-section than that of the doped quantum dots. Based on these exceptional properties, we demonstrated a flexible prototype luminescent solar concentrators using these newly synthesized doped colloidal quantum wells. These findings may open up new directions for deployment of CQWs in LSCs for advanced solar light harvesting technologies.

cond-mat.mes-hall↗