Tunable Energy Research Articles

The effect of charged particle irradiation on the transport properties of bismuth chalcogenide topological insulators: a brief review.

Topological insulators (TIs) offer a novel platform for achieving exciting applications, such as low-power electronics, spintronics, and quantum computation. Hence, the spin-momentum locked and topologically nontrivial surface state of TIs is highly coveted by the research and development industry. Particle irradiation in TIs is a fast-growing field of research owing to the industrial scalability of the particle irradiation technique. Unfortunately, real three-dimensional TI materials, such as bismuth selenide, invariably host a significant population of charged native defects, which cause the ideally insulating bulk to behave like a metal, masking the relatively weak signatures of metallic topological surface states. Particle irradiation has emerged as an effective technique for Fermi energy tuning to achieve an insulating bulk in TI along with other popularly practiced methods, such as substitution doping and electrical gating. Irradiation methods have been used for many years to enhance the thermoelectric properties of bismuth chalcogenides, predominantly by increasing carrier density. In contrast, uncovering the surface states in bismuth-based TI requires the suppression of carrier density via particle irradiation. Hence, the literature on the effect of irradiation on bismuth chalcogenides extends widely to both ends of the spectrum (thermoelectric and topological properties). This review attempts to collate the available literature on particle irradiation-driven Fermi energy tuning and the modification of topological surface states in TI. Recent studies on particle irradiation in TI have focused on precise local modifications in the TI system to induce magnetic topological ordering and surface selective topological superconductivity. Promising proposals for TI-integrated circuits have also been put forth. The eclectic range of irradiation-based studies on TI has been reviewed in this manuscript.

Unleashing the Power of Quantum Dots: Emerging Applications from Deep‐Ultraviolet Photodetectors for Brighter Futures

AbstractSince their discovery in 1981, quantum dots (QDs) have been the center of attention in optoelectronic fields owing to their excellent properties such as clearly discrete band structure, high luminous efficiency, and tunable energy bandgap via dot size control. Among them, the bandgap increase characteristic based on the quantum confinement effect opens a new horizon in the field of deep ultraviolet photodetectors (DUV PDs). Emerging applications such as risk monitoring, wireless optical communication, and chemical sensing with extremely low environmental interference raise the significance of DUV PDs. Nonetheless, the limited material selection for DUV absorption has been the main obstacle for further applications. Along this line, this review systematically revisits the recent advances in QD‐based DUV PDs, using bandgap‐widened QDs, with a focus on the synthetic method, device architecture, and interactions among constituent components. Various QDs categorized into carbon, oxide, sulfide, and nitride are reviewed with the specific characteristics of each substance. The future prospects of QD‐based DUV PDs in terms of practical applications and the current challenges are discussed.

Defect Engineering of Metal Halide Perovskite Nanocrystals via Spontaneous Diffusion of Ag Nanocrystals.

Perovskite nanocrystals (NCs) have emerged as a promising building block for the fabrication of optic-/optoelectronic-/electronic devices owing to their superior characteristics, such as high absorption coefficient, rapid ion mobilities, and tunable energy levels. However, their low structural stability and poor surface passivation have restricted their application to next-generation devices. Herein, a drug delivery system (DDS)-inspired post-treatment strategy is reported for improving their structural stability by doping of Ag into CsPbBr3 (CPB) perovskite NCs; delivery to damaged sites can promote their structural recovery slowly and uniformly, averting the permanent loss of their intrinsic characteristics. Ag NCs are designed through surface-chemistry tuning and structural engineering to enable their circulation in CPB NC dispersions, followed by their delivery to the CPB NC surface, defect-site recovery, and defect prevention. The perovskite-structure healing process through the DDS-type process (with Ag NCs as the drug) is analyzed by a combination of theoretical calculations (with density functional theory) and experimental analyses. The proposed DDS-inspired healing strategy significantly enhances the optical properties and stability of perovskite NCs, enabling the fabrication of white light-emitting diodes.

Applications of synchrotron-based X-ray diffraction in investigating thermal barrier coatings

Thermal barrier coatings play crucial roles in protecting the hot end components of aero-engines against high-temperature erosion. They must suffer extremely harsh environments including high temperatures, heavy loads, and large internal temperature gradients, which would result in various complex failures. Therefore, it is important to unveil these failure mechanisms to minimize and even prevent them for obvious reasons. Strain/stress evolution between different layers and foreign material erosion are the main failure mechanisms of thermal barrier coatings, which are well suited to be investigated using synchrotron X-ray diffraction. With its tunable energy, high flux, and many other advantages, synchrotron-based X-ray diffraction has become an advanced non-destructive characterization technique for engineering materials yielding important information including their compositions and residual stress which also provides spatial and temporal resolution that is vital for understanding their service performance. This paper presents a concise review of the applications of synchrotron-based X-ray diffraction in investigating thermal barrier coatings to explore their failure mechanisms.

What Controls Activity Trends of Electrocatalytic Water Splitting? - Activation Energy Vs. Frequency Factor

Electrocatalytic water splitting is a topic of investigation of numerous research groups for decades. Oxygen evolution reaction (OER), as a more complex and more demanding reaction, is more frequently studied, despite of the fact that the simpler hydrogen evolution reaction (HER), is generally not well understood. Nowadays, recurrent approach to electrocatalysis is conquest for more active and more stable electrode materials, very often lacking significant input to better understanding of reaction mechanisms or understanding of what are the drivers of electrocatalytic activity [1].Importantly, if one asks the key question from the conceptual point of view, and that is: what are the origins of electrocatalytic activity? - the answer will be, in the predominant majority of cases, like 70 years ago. Namely, paradigm of electrocatalysis is Sabatier principle, that suggests optimal (“not too strong, not too weak”) binding of intermediates as main precondition of high reaction rate [2]. Conventional wisdom suggests that confirmation of this should be relatively simple. Namely, Brönsted-Evans-Polanyi (BEP) relations suggest linear relationship between adsorption energy of key intermediates and activation energy. In other words, if we have reliable values of adsorption energies relevant for the electrochemical environment [3], they should form linear dependence with experimentally obtained activation energies.However, high-temperature hydrodynamic experiments on HER indicate that reducing of activation energy by tuning of adsorption energy of intermediates is not necessarily beneficial for enhancement of HER rate. Namely, HER rate is strongly influenced by preexponential frequency factor. Therefore, we propose discussion that will analyse several key aspects of HER electrocatalysis: 1) interplay of activation energy and preexponential factor as a driver of electrocatalytic activity 2) are BEP relations relevant for electrocatalysis 3) can we assess adsorption energies experimentally 4) what are relevant descriptors that shed light on HER activation process, 5) what else is important beyond Sabatier principle for rate of HER [1-7]. Figure 1. Graphical illustration of four interfacial descriptors relevant for HER. Adapted from Ref. [4] with permission from the PCCP Owner Societies, under the terms and conditions of the Creative Commons Attribution 3.0 Unported License.

Multicolor tunable luminescence and energy transfer of Tb3+/Eu3+ doped NaLaP2O7 pyrophosphate phosphors

The pyrophosphate NaLaP2O7 (NLP) samples doped with Tb3+ and Eu3+ were prepared by a simple high-temperature solid state reaction method. The XRD, SEM and spectroscopy were used for characterization. The phosphors exhibited a pure phase identified by XRD. The powders are aggregates of much smaller particles with individual sizes of about 1 μm or even smaller in diameter. The crystal structures were refined by the Rietveld method, and the unit cell parameters decreased with increasing doping concentration. The luminescence properties of the phosphors are analyzed in detail. The optimal doping concentration was determined to be 16 at.% for NLP:Tb3+ and 10 at.% for NLP:Eu3+. The color tunable luminescence from green to red was achieved by co-doping Tb3+ and Eu3+. The fluorescence dynamics fitting based on the Inokuti-Hirayama model revealed that the energy transfer mechanism is mainly contributed by the electronic dipole-dipole interaction. The energy transfer efficiency from Tb3+ to Eu3+ under 376 nm excitation is more than 50 % when the concentration of Eu3+ exceeds 10 %. Under 376 nm excitation, the emission intensity of NLP:0.16 Tb3+, 0.10Eu3+ at 423 K remains 86 % of that at room temperature, and the quantum efficiency of NLP:0.16 Tb3+, 0.10Eu3+ at room temperature is 44.29 %. The results indicate that the prepared NLP:Tb3+, Eu3+ is potential for pc-WLED applications.

(Poster Award - 2nd Place) Layer-Number Engineered Momentum-Indirect Interlayer Excitons with Large Spectral Tunability

The diversity of two-dimensional (2D) materials provides van der Waals heterostructures with abundant degrees of freedom and makes the family a promising candidate to realize novel optoelectronic devices and an attractive platform for exploring physical phenomena. Interlayer excitons in type-II van der Waals heterostructures are equipped with an oriented permanent dipole moment and long lifetime and thus would allow promising applications in excitonic and optoelectronic devices. However, in the widely studied van der Waals heterostructures constructed by transition metal dichalcogenides, the formation of interlayer excitons is limited by the lattice mismatch, rotational and translational alignment between the constituent layers, increasing the complexity of the device fabrication. Here, I will report on the robust momentum-indirect interlayer exciton emission with widely tunable emission energy via layer engineering in transition metal dichalcogenide/2D perovskite heterostructures. The transition metal dichalcogenides with different thicknesses and 2D perovskites with different layer numbers of the inorganic octahedral slabs are stacked to form type-II van der Waals heterostructures without considering special orientation arrangement and momentum mismatch. The presence of interlayer excitons is supported by the excitation-power- and temperature-dependent photoluminescence studies, photoluminescence excitation spectroscopy, time-resolved photoluminescence decay studies and electric field-dependent photoluminescence studies. Taking advantage of the thickness- or layer-number-dependence of the electronic band structure of the constituent materials, the emission energy of the interlayer excitons in our heterostructures can be tuned from 1.3 eV to 1.6 eV, providing strong evidence for the applications of van der Waals interface engineering to broad-spectrum optoelectronics. In addition, the diffusion coefficient of interlayer excitons in our heterostructures can be estimated to be ~10 cm2 s−1, which is at least one order of magnitude larger than that in the van der Waals heterostructures with Moiré superlattice, suggesting a non-localized nature that would be beneficial to the excitonic devices. Our study would offer new insights into the nature of interlayer excitons and provoke further research into their dynamics.

Sulfurization of Electrode Material: A Promising Window for Supercapacitor Technology

AbstractSupercapacitors have emerged as a promising energy storage technology with attributes like high power and tuneable energy density along with splined cyclic potential. Their performance is heavily driven by the employed electrode materials that still crave high charge storage and rate capabilities as well as virile conductivity. Among numerous applied strategies to patch the corresponding quandary, sulfurization has garnered significant attention as an effective method for improving the electrochemical depiction of electrode materials. This review article presents a comprehensive analysis of the sulfurization process applied to the electrode with the aim of providing profound overview of the latest developments, the impact of sulfur incorporation on electrode properties, and the resulting performance enhancement in supercapacitors. It explores the influence of sulfidation on the morphological, structural, and compositional aspects of electrode materials, highlighting the modification of surface area, pore size distribution, crystal structure, and the formation of active sites. The discussions on the improved specific capacitance, enhanced rate capability, prolonged cycle life, and upgraded energy density achieved are accumulated. Additionally, the review explores the challenges and limitations associated with sulfurization and strategies to mitigate trials for future directions of research and developments.

Tunable warm white light emission and energy transfer of Dy3+ co-doped Sr2 LaZrO5.5 :Eu3+ phosphors.

Eu3+ ,Dy3+ co-doped Sr2 LaZrO5.5 -based phosphors were prepared through a sol-gel method. Through characterization, it was found that the Sr2 LaZrO5.5 -based fluorescent powder co-doped with Eu3+ and Dy3+ had a cubic structure. At an excitation wavelength of 290 nm, the substrate Sr2 LaZrO5.5 exhibited strong blue emission at 468 nm, and the Sr2 LaZrO5.5 :18%Eu3+ phosphor exhibited a strong red emission peak at 612 nm. When the doping amount of Dy3+ was 5, 8, 12, 15, or 18%, the Sr2 LaZrO5.5 :18%Eu3+ phosphor changed from an orange-red light, to a warm white light, and to a cold white light. According to the emission spectra, the emission intensities of the substrates Sr2 LaZrO5.5 and Sr2 LaZrO5.5 :Eu3+ decreased with increasing Dy3+ concentration, confirming the energy transfer between the host Sr2 LaZrO5.5 -Eu3+ ,Dy3+ , and resulting in a lower CCT value, with significantly improved white light emission.

Tunable Spin-Polarized States in Graphene on a Ferrimagnetic Oxide Insulator.

Spin-polarized two-dimensional (2D) materials with large and tunable spin-splitting energy promise the field of 2D spintronics. While graphene has been a canonical 2D material, its spin properties and tunability are limited. Here, this work demonstrates the emergence of robust spin-polarization in graphene with large and tunable spin-splitting energy of up to 132 meV at zero applied magnetic fields. The spin polarization is induced through a magnetic exchange interaction between graphene and the underlying ferrimagnetic oxide insulating layer, Tm3 Fe5 O12 , as confirmed by its X-ray magnetic circular dichroism (XMCD). The spin-splitting energies are directly measured and visualized by the shift in their Landau-fan diagram mapped by analyzing the measured Shubnikov-de-Haas (SdH) oscillations as a function of applied electric fields, showing consistent fit with the first-principles and machine learning calculations. Further, the observed spin-splitting energies can be tuned over a broad range between 98 and 166 meV by field cooling. The methods and results are applicable to other 2D (magnetic) materials and heterostructures, and offer great potential for developing next-generation spin logic and memory devices.

Designing Organic and Hybrid Surfaces and Devices with Initiated Chemical Vapor Deposition (iCVD).

The initiated chemical vapor deposition (iCVD) technique is an all-dry method for designing organic and hybrid polymers. Unlike methods utilizing liquids or line-of-sight arrival, iCVD provides conformal surface modification over intricate geometries. Uniform, high-purity, and pinhole-free iCVD films can be grown with thicknesses ranging from >15µm to <5nm. The mild conditions permit damage-free growth directly onto flexible substrates, 2D materials, and liquids. Novel iCVD polymer morphologies include nanostructured surfaces, nanoporosity, and shaped particles. The well-established fundamentals of iCVD facilitate the systematic design and optimization of polymers and copolymers. The functional groups provide fine-tuning of surface energy, surface charge, and responsive behavior. Further reactions of the functional groups in the polymers can yield either surface modification, compositional gradients through the layer thickness, or complete chemical conversion of the bulk film. The iCVD polymers are integrated into multilayer device structures as desired for applications in sensing, electronics, optics, electrochemical energy storage, and biotechnology. For these devices, hybrids offer higher values of refractive index and dielectric constant. Multivinyl monomers typically produce ultrasmooth and pinhole-free and mechanically deformable layers and robust interfaces which are especially promising for electronic skins and wearable optoelectronics.

Acoustic higher-order topological states in kagome lattice with split-ring resonators

The next-nearest-neighbour (NNN) hoppings can induce many unique topological phenomena but are rarely considered in acoustics. This work investigates the higher-order topological states induced by the NNN hoppings in acoustic kagome lattice with split-ring resonators (SRRs). We build an extended tight-binding model (TBM) considering NNN hoppings to predict the topological corner modes (CMs) of the acoustic system and obtain the coupling strengths between the SRRs in different rotational angles. During rotating the SRRs, two nontrivial and one trivial systems characterized by bulk polarization can be obtained. In these two nontrivial systems, four novel CMs induced by the NNN hoppings can be observed in the first bandgap. Furthermore, the interactions between resonant and Bragg scattering effect of the SRRs are researched and the defect modes (DMs) are realized in the second bandgap. Finally, the CMs predicted by the extended TBM and DMs match well with the numerical and experimental ones. These discoveries unveil the intricate physics driven by the NNN hoppings, paving the way for innovative approaches to the design of tunable sound energy localization and multi-band metamaterials.

Metal oxide nanocrystals embedded polypyrrole nanohybrid: Exploring role of interface in photocatalytic hydrogen generation

Photocatalytic water splitting is considered as a sustainable way to produce hydrogen in the water−based energy cycle. Inorganic semiconductors, specifically metal oxides are extensively used as efficient photocatalysts, however, intrinsically poor charge-transfer and wide band gap with lower negative conduction band potential than the hydrogen evolution potential affect the water-splitting efficiency. In view of superior charge-transfer, and tunable energy levels, polymer-based nanohybrids (NHs) have been fabricated using polypyrrole (PPy) nanofibers with a series of transition metal oxides (MO) nanoparticles, namely TiO2, ZnO, CeO2, Fe2O3, NiO, and SnO2. A series of photoanodes have been tested for photoelectrochemical water splitting to elucidate the effect of interfacial charge transfer at the interfaces of NHs. The high photocurrent response of 44 μA cm−2 at 0.9 V vs. Ag/AgCl has been achieved for Fe2O3/PPy. While, ZnO/PPy NHs demonstrated a superior photocatalytic H2 generation rate of ∼162 mmol/g/h, which is ∼27 times higher than pure PPy. Based on energy level calculation, the charge transfer mechanism occurs through p−n junction in TiO2/PPy and SnO2/PPy NHs while the other NHs structures follow a Z−Scheme of charge transfer pathway. This finding opens an avenue for designing highly efficient polymer-metal oxide heterojunctions for water splitting and solar fuel applications.

Digital Mechanical Metamaterial: Encoding Mechanical Information with Graphical Stiffness Pattern for Adaptive Soft Machines.

Inspired by the adaptive features exhibited by biological organisms like the octopus, soft machines that can tune their shape and mechanical properties have shown great potential in applications involving unstructured and continuously changing environments. However, current soft machines are far from achieving the same level of adaptability as their biological counterparts, hampered by limited real-time tunability and severely deficient reprogrammable space of properties and functionalities. As a steppingstone toward fully adaptive soft robots and smart interactive machines, an encodable multifunctional material that uses graphical stiffness patterns is introduced here to in situ program versatile mechanical capabilities without requiring additional infrastructure. Through independently switching the digital binary stiffness states (soft or rigid) of individual constituent units of a simple auxetic structure with elliptical voids, in situ and gradational tunability is demonstrated here in various mechanical qualities such as shape-shifting and -memory, stress-strain response, and Poisson's ratio under compressive load as well as application-oriented functionalities such as tunable and reusable energy absorption and pressure delivery. This digitally programmable material is expected to pave the way toward multienvironment soft robots and interactive machines.

Rippled blue phosphorene with tunable energy band structures and negative Poisson’s ratio

Recent successes in the discovery of novel two-dimensional (2-D) phosphorene allotropes have motivated more in-depth investigations into tuning their properties through precise geometric control. This is also driven by the fact that these materials, particularly blue phosphorene, are highly prone to wrinkling. In this work, we systematically study the mechanical and electronic behaviors of a series of rippled blue phosphorene PN (N = 8, 18, 32, 50, 72, 98) using density functional theory combined with molecular dynamic simulations. A novel approach to tailor the electronic energy band structure of blue phosphorene is proposed by wrinkle engineering, transforming the native indirect bandgap into a direct bandgap, and enabling bandgap tuning by modifying the undulation magnitude ratio. Furthermore, the mechanical behaviors of rippled blue phosphorene differ significantly along the 4-8-4 and 4-4-4 directions. Notably, negative Poisson’s ratio is observed under tension along the 4-4-4 direction. This work demonstrates new techniques for geometrically regulating blue phosphorene and potentially other 2-D materials. The findings also yield valuable insights for the design of novel 2-D auxetic semiconductors with tunable electronic properties.

Exploring high-throughput synchrotron X-Ray powder diffraction for the structural analysis of pharmaceuticals

Synchrotron radiation offers a host of advanced properties, surpassing conventional laboratory sources with its high brightness, tunable phonon energy, photon beam coherence for advanced X-ray imaging, and a structured time profile, ideal for capturing dynamic atomic and molecular processes. However, these benefits come at the cost of operational complexity and expenses. Three decades ago, synchrotron radiation facilities, while technically open to all scientists, primarily served a limited community. Despite substantial accessibility improvements over the past two decades, synchrotron measurements still do not qualify as routine analyses. The intrinsic complexity of synchrotron science means experiments are pursued only when no alternatives suffice. In recent years, strides have been made in technology transfer offices, intermediate synchrotron-based analytical service companies, and the development of high-throughput synchrotron systems at various facilities, reshaping the perception of synchrotron science. This article investigates the practical application of synchrotron X-Ray Powder Diffraction (s-XRPD) techniques in pharmaceutical analysis. By utilizing concrete examples, we demonstrate how high-throughput systems have the potential to revolutionize s-XRPD applications in the pharmaceutical industry, rapidly generating XRPD patterns of comparable or superior quality to those obtained in state-of-the-art laboratory XRPD, all in less than 5 s. Additional cases featuring well-established pharmaceutical active ingredients (API) and excipients substantiate the concept of high throughput in pharmaceuticals, affirming data quality through structural refinements aligned with literature-derived unit cell parameters. Synchrotron data need not always be state-of-the-art to compete with lab-XRPD data. The key lies in ensuring user-friendliness, reproducibility, accessibility, cost-effectiveness, and the streamlined efforts associated with synchrotron instrumentation to remain highly competitive with their laboratory counterparts.

Unveiling the impact of exchange-correlation functionals on the description of key electronic properties of non-fullerene acceptors in organic photovoltaics.

Non-fullerene electron acceptors have emerged as promising alternatives to traditional electron-acceptors in the active layers of organic photovoltaics. This is due to their tunable energy levels, optical response in the visible light spectrum, high electron mobility, and photochemical stability. In this study, the electronic properties of two representative non-fullerene acceptors, ITIC and Y5, have been calculated within the framework of density functional theory using a range of hybrid and non-hybrid density functionals. Screened range-separated hybrid (SRSH) approaches were also tested. The results are analyzed in light of the previously reported experimental outcomes. Specifically, we have calculated the oxidation and reduction potentials, fundamental and optical gaps, the highest occupied molecular orbital and lowest unoccupied molecular orbital energies, and exciton binding energies. Additionally, we have investigated the effects of the medium dielectric constant on these properties employing a universal implicit solvent model. It was found that hybrid functionals generally perform poorly in predicting oxidation potentials, while non-hybrid functionals tend to overestimate reduction potentials. The inclusion of a large Hartree-Fock contribution to the global or long range was identified as the source of inaccuracy for many hybrid functionals in predicting both redox potentials and the fundamental and optical gaps. Corroborating with the available literature, ∼50% of all tested functionals predicted very small exciton binding energies, within the range of ±0.1eV, that become even smaller by increasing the dielectric constant of the material. Finally, the OHSE2PBE and tHCTHhyb functionals and the optimal tuning SRSH approach emerged as the best-performing methods, with good accuracy in the description of the electronic properties of interest.

Biaxial strain tuning of exciton energy and polarization in monolayer WS2

We perform micro-photoluminescence and Raman experiments to examine the impact of biaxial tensile strain on the optical properties of WS2 monolayers. A strong shift on the order of −130 meV per % of strain is observed in the neutral exciton emission at room temperature. Under near-resonant excitation, we measure a monotonic decrease in the circular polarization degree under the applied strain. We experimentally separate the effect of the strain-induced energy detuning and evaluate the pure effect coming from the biaxial strain. The analysis shows that the suppression of the circular polarization degree under the biaxial strain is related to an interplay of energy and polarization relaxation channels as well as to variations in the exciton oscillator strength affecting the long-range exchange interaction.

Tunable and recoverable energy absorption of foam-embedded architected cellular composite material at multiple strain rates

Cellular multistable architected material has been widely studied for its promising energy absorption applications for personnel protection, protective packaging, and crash mitigation. Despite the tailorable properties enabled by their geometric features, a major issue in the actual application is their lower strengths in the elastic behavior of the multistable architected material. Herein, a novel design strategy of strain rate-dependent architected cellular composite material (FACCM) is proposed, aiming to achieve enhanced energy-absorbing properties with the proposed composite system than the single material constituent. Guided by numerical simulations and experimental tests, the compressive behaviour of FACCM at multiple strain rates and the effect of filled foam on it with specific geometric parameters are characterized. The quasi-static performances of the FACCM specimens were evaluated both at the cell level and planar array level. Our results indicate that the strength, stiffness, and snap-through behaviour of multistable architected material can be significantly improved by the filled foam at elevated loading rates regardless of quasi-static loading or impact tests. The current study offers a new strategy for developing novel packing, shock absorption, and impact protection systems.

Distinct Excitonic Emissions in 2D (C7 H7 N2 )2 PbX4 (X=Cl, Br) under Compression.

Two dimensional (2D) hybrid metal halides (HMHs) usually exhibit free excitonic (FE) emission, and self-trapped excitonic (STE) emission can also be achieved by adopting appropriate halogens and organic cations. Recently, significant efforts have been made to modulate and then clarify the transformation and connection between these two types of excitonic emissions in 2D HMHs. In this study, intriguing pressure-tuned transitions between FE emission and STE emission are observed in 2D (C7 H7 N2 )2 PbCl4 . In contrast, only FE emissions with tunable emission energies are observed in 2D (C7 H7 N2 )2 PbBr4 which possesses a similar structure with (C7 H7 N2 )2 PbCl4 under compression. Such distinct halide-dependent optical responses under pressure are experimentally revealed to arise from the intricate interplay among several factors in these HMHs, including the stiffness of the structure, the Coulomb force between the organic cations and the inorganic octahedra, and the magnitude of inorganic octahedral distortion. These high-pressure optical explorations can unravel the underlying interrelationship between the crystal structure and excitonic emission in 2D HMHs.