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In this talk, we show that the phenomenon known as &quot;Valley Hall Effect&quot;, whereby a an electric field induces a transverse valley current, is better described as an instance of the Orbital Hall Effect (OHE), where the ambiguous ``valley&#39;&#39; indices are replaced by a physical quantity, the orbital magnetic moment, which can be defined uniformly over the entire Brillouin zone. This description removes ambiguities that are present in the definition of the valley Hall current, as the conductivity in the orbital Hall effect is unambiguously defined as the Brillouin zone integral of a new quantity, called the orbital Berry curvature. The reformulation in terms of OHE is illustrated in the case of gapped graphene, which has been previously proposed to be a good platform to observe the valley Hall effect. The new formulation provides a direct explanation to the orbital moments accumulated at the edges of the sample, which were observed in previous Kerr rotation measurements.


MATERIALS FOR HUMANITY (MH 21)

Orbital Hall effect as an alternative to valley Hall effect in gapped graphene

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In this talk, we show that the phenomenon known as "Valley Hall Effect", whereby a an electric field induces a transverse valley current, is better described as an instance of the Orbital Hall Effect (OHE), where the ambiguous ``valley'' indices are replaced by a physical quantity, the orbital magnetic moment, which can be defined uniformly over the entire Brillouin zone. This description removes ambiguities that are present in the definition of the valley Hall current, as the conductivity in the orbital Hall effect is unambiguously defined as the Brillouin zone integral of a new quantity, called the orbital Berry curvature. The reformulation in terms of OHE is illustrated in the case of gapped graphene, which has been previously proposed to be a good platform to observe the valley Hall effect. The new formulation provides a direct explanation to the orbital moments accumulated at the edges of the sample, which were observed in previous Kerr rotation measurements.


technical paper

It is known that quantum phenomena become more pronounced in materials with reduced dimensionalities. The family of two-dimensional (2D) transition metal dichalcogenides (TMDs) exhibit a host of emergent quantum phenomena, such as valley-selective optical selection rules, the fractional quantum Hall effect and single photon emission. In this talk, we present insights from recent first principles calculations that map the atomic and electronic structure of 2D TMD materials to observable quantum phenomena. Using first principles calculations without any empirical parameters, we predict the Landau levels as well as single-band and exciton g-factors for 2D semiconducting H-phase TMDs, and elucidate the role of many-body interactions in the Zeeman effect [1]. We further present the optical properties of defect-induced localized excitons in these TMD materials, which are of relevance to single photon emission and quantum photonics applications [2]. Finally, we discuss how many-body interactions and interfacial hybridization can lead to spin-dependent tunneling barriers in cobalt pthalocyanine molecules adsorbed on the 2D TMD, VSe2 [3].

[1] Physical Review Research, 2, 033256 (2020)
[2] ACS Nano 13, 6050 (2019)
[3] J Phys Chem Lett 11, 9358 (2020)


Valleytronics, Quantum Photonics and Spintronics in Two-Dimensional Transition Metal Dichalcogenides

Electron emission from a surface or charge injection across an interface is a fundamental process in electronics and photonics. Depending on the energy involved, it can be broadly characterized into 3 different processes known as thermionic emission TE (by thermal energy), field emission FE (by quantum tunneling) and photoemission PE (by absorption of photons or optical tunneling). When the amount of charge is sufficient high, it will affect the space charge field that the process will saturated. With the development of new quantum materials including two-dimensional (2D) materials and 2D/3D Topological semi-metals, many classical laws or models will require revisions to account for new material properties, as well as novel operating regimes in nanometer dimensions and in ultrashort time scales. Thus the basic interaction of electrons between these quantum materials should be studied carefully before wrongly use the classical models directly. In this talk, some recent and self-consistent models will be presented, with applications related to electronics and photonics. These new models exhibit smooth transition to the classical models, report new findings to explain some experimental results, and to predict new operating regimes.

Charge injection and its interaction with quantum materials

Over the last two decades, prototype devices for future classical and quantum computing technologies have been fabricated by using scanning tunnelling microscopy and hydrogen resist lithography to position phosphorus atoms in silicon with atomic-scale precision. Despite these successes, it is only recently that our group demonstrated that a donor precursor molecule other than phosphine is compatible with the hydrogen resist lithography technique [1]. Here we describe the successful fabrication of atomic-scale structures of arsenic-in-silicon, using arsine (AsH3) as the precursor molecule. We fully elucidate the surface chemistry and reaction pathways of arsine on Si(001), revealing significant differences to phosphine. The properties of arsenic-in-silicon devices, and potential benefits of using arsenic instead of phosphorus, are briefly highlighted using spectroscopic and electrical characterisation techniques. Also presented will be recent work showing that broadband electric force microscopy (bb-EFM) can be used to characterise the properties of a nanoscale p-n junction [2], made from phosphorus and boron using hydrogen lithography by our collaborators at IBM Research - Zürich.
[1] T.J.Z. Stock et al., ACS Nano, 14 3316 (2020).
[2] G. Gramse et al., Nature Electronics, 3 531 (2020).


Fabrication and characterisation of nano- and atomic-scale dopant structures in silicon

Recent progress on activatable fluorescent imaging probes and photosensitizers

Switchable phototheranostic nanomaterials are of particular interest for specific biosensing, high-quality imaging, and targeted therapy in the field of precision nanomedicine. Here, we develop a “one-for-all” nanomaterial (NanoPcTBs) that self-assembles from flexible and versatile phthalocyanine building blocks. Fluorescence and reactive oxygen species (ROS) generation could be triggered depending on a targeted, protein-induced, partial disassembly mechanism, which creates opportunities for low-background fluorescence imaging and activatable photodynamic therapy (PDT).1,2 
On the othet hand, the development of activatable and responsive optical probes is contributing to a better understanding of oncogenesis at the molecular level. Monitoring fluctuations in enzyme overexpression facilitates early tumors detection and excision. Relying on abnormal alkaline phosphatase (ALP) activity, DQM-ALP was successfully used to differentiate between tumors tissues and normal tissues in nude BABL/c mice bearing HepG-2 and HeLa xenograft tumors.3 In addition, a near-infrared two-photon fluorescent probe was developed to not only specially image carboxylesterase (CE) activity in vivo and in situ but also target orthotopic liver tumor after systemic administration.4

References

1. X. Li, S. Yu, Y. Lee, T. Guo, N. Kwon, D. Lee, S. C. Yeom, Y. Cho, G. Kim, J.-D. Huang, S. Choi, K. T. Nam, J. Yoon, J. Am. Chem. Soc. 2019, 141, 1366-1372.
2. H.-B. Cheng, B. Qiao, H. Li, J. Cao, Y. Luo, K. M. K. Swamy, J. Zhao, Z. Wang, J. Y. Lee, X.-J. Liang, J. Yoon, J. Am. Chem. Soc. 2021, 143, 2413-2422.
3. H. Li, Q. Yao, F. Xu, Y. Li, D. Kim, J. Chung, G. Baek, X. Wu, P. F. Hillman, E. Y. Lee, H. Ge, J. Fan, J. Wang, S.-J. Nam, X. Peng, J. Yoon, Angew. Chem. Int. Ed. 2020, 59, 10186-10195.
4. X. Wu, R. Wang, S. Qi, N. Kwon, J. Han, H. Kim, H. Li, F. Yu, J. Yoon, Angew. Chem. Int. Ed. 2021, 60, doi.org/10.1002/anie.202101190.


Recent progress on activatable fluorescent imaging probes and photosensitizers

Inspired by Natural biomineralization processes, our research focuses on the rational design of peptide- and nucleic acid-based biomolecular templates for the synthesis of multifunctional metallic and carbon-based nanomaterials with tunable optical properties and biofunctionalities for sensing, imaging, drug/gene delivery and therapy. Such bio-hybrid nanomaterials exhibit synergistic combination of biological functions and chemical properties resulting from the hard nanocore and soft biomolecular shell. For example, we have developed a series of metallic nanobiosensors with target specific bio-shell to detect wide range of analytes in solution from small molecule drugs, protein biomarkers to cancer and bacteria cells [1-4]. Recently, we have exploited the use of designer DNA and peptide templates to synthesize a palette of photoluminescent metal nanoclusters (NCs < 2nm in core size) which could be used as multicolour probes for bioimaging, image-guided photodynamic therapy and multiplexed sensing [5-7]. We also take this biomimetic approach to ‘turn’ the native protein into bioactive fluorescent nanosensor for rapid drug screening without tedious genetic engineering. To enable greener synthesis with good biocompatibility and sustainability, pure organic resources and biomass wastes were utilized to synthesize carbon dots from biomolecules (biodots) and metal-enhanced fluorescent nanodots with tailored functionalities for a range of biomedical applications [8-12]. For instance, bioinspired antimicrobial biodots has been successfully developed for ultrasensitive pathogen detection (1 cfu/ml in < 0.5 hour) as well as to combat broad spectrum multi-drug resistant bacteria [11]. With further understanding in biotemplates design, we expect a far more extensive applications of bioinspired hybrid nanomaterials for the advanced biomedical diagnostic and treatment towards personalized nanomedicine in future.

Bioinspired Nanomaterials for Biomedical Diagnostics and Treatment Towards Personalized Nanomedicine

Seeing the Sound: Optical Neural Interfaces for In Vivo Neuromodulation

Light plays vital roles in organisms for manipulating a variety of important biological processes because of its high degree of spatiotemporal resolution and ease of precisely regulating parameters. Studying biological pathways underlying diseased states always requires bidirectional controlling over the signal processes. To allow programmable or bidirectional regulations of multiple biological pathways, probes should exhibit orthogonal emission properties with modulation of external stimuli such as excitation wavelength. The complicated energy level structure of lanthanide ions can be an asset to achieve such multi-coloured emission, if one can precisely navigate the energy transfer pathways within single lanthanide ions to favour discrete energy transitions. This challenge once overcome would eliminate the need for using multiple lanthanide ions for obtaining orthogonal emissive properties. For example, Er3+ ions are able to produce green color luminescence through the 2H11/2, 4S3/2→4I15/2 transition, and red emission from the 4F9/2→4I15/2 transition. We have explored cross-relaxation to manipulate energy migration within the same lanthanide activator ion (Er3+) in upconversion nanoparticles (UCNPs) to produce orthogonal red and green emissions, simply by adjusting the excitation wavelength from 980 nm to 808 nm. These UCNPs offer a powerful tool for programmable activation of two synergistic light gated ion channels VChR1 and Jaws in the same cell to manipulate membrane depolarization and hyperpolarization for a multitude of disease therapies, demonstrated here for cardiac pacing. Moreover, this orthogonal emissive UCNP was designed to develop single-line based test strip, in which one emission can be used as reporting signal, and another one as calibrating signal. Due to the removal of control lines, such novel strategy greatly reduces strip size, facilitating design a testing array for multiple detections of different samples.

Orthogonal Upconversion Luminescence from Single Lanthanide Activator Ion for Disease Diagnosis

Dental caries remains a persistent major oral healthcare burden worldwide with little significant improvement in dental healthcare in the last 30 years. Intraoral/biofilm-tooth pH is the single parameter that has demonstrated accurate assessment of the caries risk, reflecting the summative integrated outcome of the complicated interactions between the three etiological factors, namely microorganisms/biofilm, diet/carbohydrates, and tooth/saliva/host. However, there is no technology/system capable of probing both the micro-pH profile in dentin tissue and acidogenic oral biofilm simultaneously, with high spatial/temporal resolution of pathophysiologic acid attacks. Herein, a highly sensitive pH-responsive Hybrid NanoParticle (pH-NP) is developed coupled with an ex vivo tooth-biofilm caries model to simulate key cariogenic determinants/steps in a well-controlled platform to decipher the mechanistic complexity of caries initiation/formation. The pH-NP emits two fluorescence intensities that can change in opposite directions with pH to measure with a ratiometric output sensitivity of 13.4-fold a broad clinically-relevant pH range of 3.0–8.0. Using [H+], in addition to pH, to calculate the “area-under-curve” corroborates with the “minimum-pH” in semi-quantifying the demineralizing potential in each biofilm-dentin zones/depth. The data mechanistically elucidates a two-pronged cariogenic effect of a popular-acidic-sweet-drink, in inundating the biofilm/tooth-system with H+ from both the drink and the metabolic by-products of biofilm.

Imaging Spatiotemporal pH Changes in Biofilm-Dentin Microenvironments using pH-Responsive Hybrid Nanoparticles

Targeting Inflammatory Macrophages with Polysaccharide Nanocarriers

Thermogels are valuable soft materials for biomedical applications. At low temperatures, they remain as solutions which can be used to entrap therapeutic payloads such as drugs and proteins within their solvated polymer matrices. Upon injection into the body, higher body temperatures cause the solutions to gelate in situ at the site of injection, allowing localized placement for applications such as drug delivery. Herein, we present our three-component thermogelling polyurethane technology comprising of biocompatible polyethylene glycol (PEG), poly(propylene glycol) (PPG) and a third component, which can be poly(caprolactone) (PCL), poly(tetrahydrofuran) carbonate (PTHF) or poly[(R)-3-hydroxybutyrate-(R)-3-hydroxyhexanoate] (PHBHx), as a unique platform for biomedical applications. Our thermogels loaded with anticancer drugs were highly effective for inhibition of tumour growth in vivo using mice models. Docetaxel-loaded PEG-PPG-PHBHx thermogels showed enhanced anti-melanoma effects on solid melanoma tumours compared with the free drug, whilst exhibiting excellent biosafety and no apparent harm to organs. With doxorubicin-loaded PEG-PPG-PTHF thermogels, sustained drug release for 16 days in vivo successfully inhibited growth of hepatocellular carcinoma. Impressively, incorporating a dye capable of aggregation-induced emission into the polymer structure allowed it to be used to track in-vivo doxorubicin release status and gel degradation, revealing valuable insights on the drug transportation pathways. Recent efforts on PEG-PPG-PCL thermogels are concentrated on their unprecedented use in vitreoretinal surgery as a vitreous substitute and an internal tamponading agent. The thermogel showed long-term biocompatibility in rabbit vitrectomy models, and was an effective endotamponade in a non-human primate surgical retinal detachment model. This is likely attributed to the thermogel providing support for the retina and preventing subsequent re-detachments.

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Orbital Hall effect as an alternative to valley Hall effect in gapped graphene

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