arXiv subjects

Tze Chien Sum

Publications and source records attributed to Tze Chien Sum.

12 recordsLinked to original sources

arXiv2026

Bandedge-state-limited single-photon emission from volumetric quantum design of 2D colloidal quantum wells

Present-day solution-processable single-photon sources are dominated by three-dimensionally confined colloidal quantum dot emitters, yet their particle-to-particle variation in single-exciton properties limits reproducibility and scalability. Here, to avoid such heterogeneity, we demonstrate reliable room-temperature single-photon emission from atomically flat two-dimensional (2D) colloidal quantum wells (CQWs) with inherently uniform one-dimensional quantum confinement, despite their long-standing limitations of efficient multiexciton emission and pronounced exciton-surface susceptibility. We resolve these challenges through volumetric quantum design (VQD) of CQWs, yielding a highly localized, single bandedge state. This design laterally confines the bandedge excitonic domain within the exciton coherent area and vertically decouples it from surface states via a thick, strain-relieved quantum-barrier shell that preserves strong confinement, overcoming the daunting thickness-confinement trade-off in 2D CQWs. Statistical single-particle spectroscopy reveals that VQD-CQWs deliver near-blinking-free (on-time >99.5%) and fluence-insensitive antibunching (g(2)(0): 0.041), protected by a bandedge-state-filling bottleneck, together with linear polarization of up to 73% under cavity-free conditions, originating from synergistic transition-dipole and electric-field anisotropies. These advances establish 2D CQWs as a viable, homogenous and scalable platform for quantum technologies.

physics.app-ph↗

arXiv2025

Quotient Complex Transformer (QCformer) for Perovskite Data Analysis

The discovery of novel functional materials is crucial in addressing the challenges of sustainable energy generation and climate change. Hybrid organic-inorganic perovskites (HOIPs) have gained attention for their exceptional optoelectronic properties in photovoltaics. Recently, geometric deep learning, particularly graph neural networks (GNNs), has shown strong potential in predicting material properties and guiding material design. However, traditional GNNs often struggle to capture the periodic structures and higher-order interactions prevalent in such systems. To address these limitations, we propose a novel representation based on quotient complexes (QCs) and introduce the Quotient Complex Transformer (QCformer) for material property prediction. A material structure is modeled as a quotient complex, which encodes both pairwise and many-body interactions via simplices of varying dimensions and captures material periodicity through a quotient operation. Our model leverages higher-order features defined on simplices and processes them using a simplex-based Transformer module. We pretrain QCformer on benchmark datasets such as the Materials Project and JARVIS, and fine-tune it on HOIP datasets. The results show that QCformer outperforms state-of-the-art models in HOIP property prediction, demonstrating its effectiveness. The quotient complex representation and QCformer model together contribute a powerful new tool for predictive modeling of perovskite materials.

cs.LG↗

arXiv2024

Quotient complex (QC)-based machine learning for 2D perovskite design

With remarkable stability and exceptional optoelectronic properties, two-dimensional (2D) halide layered perovskites hold immense promise for revolutionizing photovoltaic technology. Presently, inadequate representations have substantially impeded the design and discovery of 2D perovskites. In this context, we introduce a novel computational topology framework termed the quotient complex (QC), which serves as the foundation for the material representation. Our QC-based features are seamlessly integrated with learning models for the advancement of 2D perovskite design. At the heart of this framework lies the quotient complex descriptors (QCDs), representing a quotient variation of simplicial complexes derived from materials unit cell and periodic boundary conditions. Differing from prior material representations, this approach encodes higher-order interactions and periodicity information simultaneously. Based on the well-established New Materials for Solar Energetics (NMSE) databank, our QC-based machine learning models exhibit superior performance against all existing counterparts. This underscores the paramount role of periodicity information in predicting material functionality, while also showcasing the remarkable efficiency of the QC-based model in characterizing materials structural attributes.

cs.CE↗

arXiv2023

Dicke superradiance requires interactions beyond nearest-neighbors

Photon-mediated interactions within an excited ensemble of emitters can result in Dicke superradiance, where the emission rate is greatly enhanced, manifesting as a high-intensity burst at short times. The superradiant burst is most commonly observed in systems with long-range interactions between the emitters, although the minimal interaction range remains unknown. Here, we put forward a new theoretical method to bound the maximum emission rate by upper bounding the spectral radius of an auxiliary Hamiltonian. We harness this tool to prove that for an arbitrary ordered array with only nearest-neighbor interactions in all dimensions, a superradiant burst is not physically observable. We show that Dicke superradiance requires minimally the inclusion of next-nearest-neighbor interactions. For exponentially decaying interactions, the critical coupling is found to be asymptotically independent of the number of emitters in all dimensions, thereby defining the threshold interaction range where the collective enhancement balances out the decoherence effects. Our findings provide key physical insights to the understanding of collective decay in many-body quantum systems, and the designing of superradiant emission in physical systems for applications such as energy harvesting and quantum sensing.

quant-ph↗

arXiv2021

Pseudo-magnetic field-induced ultra-slow carrier dynamics in periodically strained graphene

The creation of pseudo-magnetic fields in strained graphene has emerged as a promising route to allow observing intriguing physical phenomena that would be unattainable with laboratory superconducting magnets. Scanning tunneling spectroscopy experiments have successfully measured the pseudo-Landau levels and proved the existence of pseudo-magnetic fields in various strained graphene systems. These giant pseudo-magnetic fields observed in highly deformed graphene can substantially alter the optical properties of graphene beyond a level that can be feasible with an external magnetic field, but the experimental signatures of the influence of such pseudo-magnetic fields have yet to be unveiled. Here, using time-resolved infrared pump-probe spectroscopy, we provide unambiguous evidence for ultra-slow carrier dynamics enabled by pseudo-magnetic fields in periodically strained graphene. Strong pseudo-magnetic fields of ~100 T created by non-uniform strain in graphene nanopillars are found to significantly decelerate the relaxation processes of hot carriers by more than an order of magnitude. Our finding presents unforeseen opportunities for harnessing the new physics of graphene enabled by pseudo-magnetic fields for optoelectronics and condensed matter physics.

cond-mat.mes-hall↗

arXiv2021

Room Temperature Light-Mediated Long-Range Coupling of Excitons in Perovskites

Perovskites have been the focus of attention due to their multitude of outstanding optoelectronic properties and structural versatility. Two-dimensional halide perovskite such as (C_6H_5C_2H_4NH_3)_2PbI_4, or simply PEPI, forms natural multiple quantum wells with enhanced light-matter interactions, making them attractive systems for further investigation. This work reports tunable splitting of exciton modes in PEPI resulting from strong light-matter interactions, manifested as multiple dips (modes) in the reflection spectra. While the origin of the redder mode is well understood, that for the bluer dip at room temperature is still lacking. Here, it is revealed that the presence of the multiple modes originates from an indirect coupling between excitons in different quantum wells. The long-range characteristic of the mediated coupling between excitons in distant quantum wells is also demonstrated in a structure design along with its tunability. Moreover, a device architecture involving an end silver layer enhances the two excitonic modes and provides further tunability. Importantly, this work will motivate the possibility of coupling of the excitonic modes with a confined light mode in a microcavity to produce multiple exciton-polariton modes.

cond-mat.mtrl-sci↗

arXiv2020

Efficacious symmetry-adapted atomic displacement method for lattice dynamical studies

Small displacement methods have been successfully used to calculate the lattice dynamical properties of crystals. It involves displacing atoms by a small amount in order to calculate the induced forces on all atoms in a supercell for the computation of force constants. Even though these methods are widely in use, to our knowledge, there is no systematic discussion of optimal displacement directions from the crystal's symmetry point of view nor a rigorous error analysis of such methods. Based on the group theory and point group symmetry of a crystal, we propose displacement directions, with an equivalent concept of the group of $k$, deduced directly in the Cartesian coordinates rather than the usual fractional coordinates, that maintain the theoretical maximum for the triple product $V$ spanned by the three displacements to avoid possible severe roundoff errors. The proposed displacement directions are generated from a minimal set of irreducible atomic displacements that keep the required independent force calculations to a minimum. We find the error in the calculated force constant explicitly depends on the inverse of $V$ and inaccuracy of the forces. Test systems such as Si, graphene, and orthorhombic Sb2S3 are used to illustrate the method. Our displacement method is shown to be very robust in treating low-symmetry cells with a large `aspect ratio' due to huge differences in lattice parameters, use of a large vacuum height, or a very oblique unit cell due to unconventional choice of primitive lattice vectors. It is expected that our displacement strategy can be used to address higher-order interatomic interactions to achieve good accuracy and efficiency.

cond-mat.mtrl-sci↗

arXiv2020

Zone-folded longnitude acoustic phonons driving self-trapped state emission in colloidal CdSe nanoplate superlattice

Colloidal cadmium chalcogenide nanoplates are two-dimensional semiconductors that have shown great application prospect for light-emitting technologies. Self-trapped state (STS), a special localized state originated from strong electron-phonon coupling (EPC), has great potential in one-step white light luminance owing to its broadband emission linewidth. However, achieving STS in cadmium chalcogenide nanocrystals is extremely challenging due to their intrinic weak EPC nature. By building hybrid superlattice (SL) structures via self-assembly of colloidal CdSe nanoplates (NPLs), we demonstrated an emergence of zone-folded longnitude acoustic phonons (ZFLAP) differ from monodispersed NPLs, and observed a broadband STS emission in spectra range of 450-600 nm. Through femtosecond transient absorption and impulsive vibrational spectroscopy, we revealed that STS is generated in time scale of ~500 fs and is driven by strong coupling of excitons and ZFLAPs with Huang-Rhys parameter as large as ~22.7. Our findings provide a new avenue for generating and manipulating STS emission by artificially designing and building hybrid periodic structures superior to single material optimization.

cond-mat.mtrl-sci↗

arXiv2019

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↗

arXiv2018

Room Temperature Continuous-wave Excited Biexciton Emission in CsPbBr3 Nanocrystals

Biexcitons are a manifestation of many-body excitonic interactions crucial for quantum information and quantum computation in the construction of coherent combinations of quantum states. However, due to their small binding energy and low transition efficiency, most biexcitons in conventional semiconductors exist either at cryogenic temperature or under femtosecond pulse laser excitation. Here we demonstrate room temperature, continuous wave driven biexciton states in CsPbBr3 perovskite nanocrystals through coupling with a plasmonic nanogap. The room temperature CsPbBr3 biexciton excitation fluence (~100 mW/cm2) is reduced by ~10^13 times in the Ag nanowire-film nanogaps. The giant enhancement of biexciton emission is driven by coherent biexciton-plasmon Fano interference. These results provide new pathways to develop high efficiency non-blinking single photon sources, entangled light sources and lasers based on biexciton states.

cond-mat.mes-hall↗

arXiv2015

Controlled Synthesis of Organic/Inorganic van der Waals Solid for Tunable Light-matter Interactions

Van der Waals (vdW) solids, as a new type of artificial materials that consist of alternating layers bonded by weak interactions, have shed light on fascinating optoelectronic device concepts. As a result, a large variety of vdW devices have been engineered via layer-by-layer stacking of two-dimensional materials, although shadowed by the difficulties of fabrication. Alternatively, direct growth of vdW solids has proven as a scalable and swift way, highlighted by the successful synthesis of graphene/h-BN and transition metal dichalcogenides (TMDs) vertical heterostructures from controlled vapor deposition. Here, we realize high-quality organic and inorganic vdW solids, using methylammonium lead halide (CH3NH3PbI3) as the organic part (organic perovskite) and 2D inorganic monolayers as counterparts. By stacking on various 2D monolayers, the vdW solids behave dramatically different in light emission. Our studies demonstrate that h-BN monolayer is a great complement to organic perovskite for preserving its original optical properties. As a result, organic/h-BN vdW solid arrays are patterned for red light emitting. This work paves the way for designing unprecedented vdW solids with great potential for a wide spectrum of applications in optoelectronics.

physics.chem-ph↗

arXiv2014

First-principles study of the lattice dynamics of Sb2S3

We present a lattice dynamics study of orthorhombic antimony sulphide (Sb2S3) obtained using density-functional calculations in conjunction with the supercell force-constant method. The effect of Born effective charges is taken into account using a mixed-space approach, resulting in the splitting of longitudinal and transverse optical (LO-TO) phonon branches near the zone center. Zone-center frequencies agree well with Raman scattering experiments. Due to the slow decay of the interatomic force constants (IFC), a minimal 2x4x2 supercell (Pnma setting) with 320 atoms is crucial for an accurate determination of the dispersion relations. Smaller supercells result in artificial acoustic phonon softening and unphysical lifting of degeneracies along high symmetry directions. We propose a scheme to investigate the convergence of the IFC with respect to the supercell sizes. The phonon softening can be attributed to the periodic images that affect the accuracy of the force constants, and the truncation of long-ranged forces. The commensuration of the q-vectors with the supercell size is crucial to preserve degeneracies in Sb2S3 crystals.

cond-mat.mtrl-sci↗