arXiv subjects

Khalid M. Siddiqui

Publications and source records attributed to Khalid M. Siddiqui.

7 recordsLinked to original sources

arXiv2026

Electron coherent phonon coupling in Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ measured with ultrafast broadband spectroscopy

Photoexcitation of single-layered La$_{0.5}$Mn$_{1.5}$MnO$_4$ has played a key role in understanding orbital ordering and non-thermal states in the manganites. However, while orbital ordering in La$_{0.5}$Sr$_{1.5}$MnO$_4$ breaks the in-plane C$_4$ symmetry, many layered manganites show much more complex phase diagrams in which orbital ordering emerges from an already symmetry-broken high-temperature phase and also exhibit additional low-temperature phases. In this work, we examine the role of these phases in relation to orbital ordering in the single-layered manganite Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ with a combination of optical reflection anisotropy and ultrafast broadband pump-probe spectroscopy. We find that the reflection anisotropy, measured in equilibrium, is strongly sensitive to charge and orbital-ordering transition only. However, the ultrafast response, measuring the non-equilibrium state is sensitive to all phases. In particular, we deduce that coherent phonons modulate unoccupied electronic states that are sensitive to the different phases of the material. This gives rise to a non-linear scaling of the phonon signal with pump fluence at specific probe wavelengths.

cond-mat.str-el↗

arXiv2025

A versatile setup for symmetry-resolved ultrafast dynamics of quantum materials

Correlated phenomena occur in quantum materials because of the delicate interplay between internal degrees of freedom, leading to multiple symmetry-broken quantum phases. Resolving the structure of these phases is a key challenge, often requiring facilities equipped with x-ray free-electron lasers and electron sources that may not be readily accessible to the average user. Table-top sources that offer alternative means are therefore needed. In this work, we present an all-optical, table-top setup that enables symmetry-resolved studies using linear and nonlinear spectroscopies. We demonstrate the versatility of the setup with chosen examples that underscore the importance of tracking symmetries and showcase the strengths of the setup, which offers a large tunable parameter space.

cond-mat.str-el↗

arXiv2025

Ultrafast surface melting of orbital order in La0.5Sr1.5MnO4

Understanding how light modifies long-range order in quantum materials is key to improving our ability to control functionality. However, this is challenging if the response is heterogeneous. Here we address the most common form of light-induced heterogeneity, surface melting, and measure the dynamics of orbital order in the layered manganite, La0.5Sr1.5MnO4. We isolate the surface dynamics from the bulk by measuring the orbital truncation rod as well as orbital Bragg peak. After photoexcitation, the orbital Bragg peak shows an unusual narrowing, which suggests an increase in the correlation length in the probed volume. In contrast, the correlation length at the surface decreases. These differences can be reconciled if the material is heterogeneous, and light melts a less ordered surface. By isolating the surface response, we determine that the loss of long-range order is an incoherent process, which is likely accompanied by the formation of local polarons.

cond-mat.str-el↗

arXiv2023

Determination and correction of spectral phase from principal component analysis of coherent phonons

Measuring the spectral phase of a pulse is key for performing wavelength resolved ultrafast measurements in the few femtosecond regime. However, accurate measurements in real experimental conditions can be challenging. We show that the reflectivity change induced by coherent phonons in a quantum material can be used to infer the spectral phase of an optical probe pulse with few-femtosecond accuracy.

physics.optics↗

arXiv2023

Ultrafast X-ray imaging of the light-induced phase transition in VO2

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

cond-mat.str-el↗

arXiv2023

Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, we examine ultrafast laser heating of single-crystal gold films. Comparison of kinematical and dynamical models reveals the strong effects of dynamical scattering within nm-scale films and their dependence on sample topography and probe kinetic energy. Applying to UED experiments on an 11 nm thick film using 750 keV electron probe pulses, the dynamical models provide a tenfold improvement over a comparable kinematical model in matching the measured UED patterns. Also, the retrieved lattice temperature rise is in very good agreement with predictions based on previously measured optical constants of gold, whereas fitting the Debye-Waller factor retrieves values that are more than three times lower. Altogether, these results show the importance of dynamical scattering theory for quantitative analysis of UED and demonstrate models that can be practically applied to single-crystal materials and heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast optical melting of trimer superstructure in layered 1T'-TaTe2

Quasi-two-dimensional transition-metal dichalcogenides are a key platform for exploring emergent nanoscale phenomena arising from complex interactions. Access to the underlying degrees-of-freedom on their natural time scales motivates the use of advanced ultrafast probes sensitive to self-organised atomic-scale patterns. Here, we report the first ultrafast investigation of TaTe2, which exhibits unique charge and lattice trimer order characterised by a transition upon cooling from stripe-like chains into a $(3 \times 3)$ superstructure of trimer clusters. Utilising MeV-scale ultrafast electron diffraction, we capture the photo-induced TaTe2 structural dynamics -- exposing a rapid $\approx\!1.4$ ps melting of its low-temperature ordered state followed by recovery via thermalisation into a hot cluster superstructure. Density-functional calculations indicate that the initial quench is triggered by intra-trimer Ta charge transfer which destabilises the clusters, unlike melting of charge density waves in other TaX2 compounds. Our work paves the way for further exploration and ultimately rapid optical and electronic manipulation of trimer superstructures.

cond-mat.mtrl-sci↗