The recently demonstrated chiral modes of lattice motion carry angular momentum and therefore directly couple to magnetic fields. Notably, their magnetic moments are predicted to be strongly influenced by electronic contributions. Here, we have studied the magnetic response of transverse optical phonons in a set of Pb1−xSnxTe films, which is a topological crystalline insulator forx> 0.32 and has a ferroelectric transition at anx-dependent critical temperature. Polarization-dependent terahertz magnetospectroscopy measurements revealed Zeeman splittings and diamagnetic shifts, demonstrating a large phonon magnetic moment. Films in the topological phase exhibited phonon magnetic moment values that were larger than those in the topologically trivial samples by two orders of magnitude. Furthermore, the sign of the effective phonong-factor was opposite in the two phases, a signature of the topological transition according to our model. These results strongly indicate the existence of interplay between the magnetic properties of chiral phonons and the topology of the electronic band structure.
more »
« less
This content will become publicly available on January 31, 2026
Transforming achiral semiconductors into chiral domains with exceptional circular dichroism
Highly concentrated solutions of asymmetric semiconductor magic-sized clusters (MSCs) of cadmium sulfide, cadmium selenide, and cadmium telluride were directed through a controlled drying meniscus front, resulting in the formation of chiral MSC assemblies. This process aligned their transition dipole moments and produced chiroptic films with exceptionally strong circular dichroism.G-factors reached magnitudes as high as 1.30 for drop-cast films and 1.06 for patterned films, approaching theoretical limits. By controlling the evaporation geometry, various domain shapes and sizes were achieved, with homochiral domains exceeding 6 square millimeters that transition smoothly between left- and right-handed chirality. Our results uncovered fundamental relationships between meniscus deposition processes, the alignment of supramolecular filaments and their MSC constituents, and their connection to emergent chiral properties.
more »
« less
- PAR ID:
- 10577342
- Publisher / Repository:
- AAAS
- Date Published:
- Journal Name:
- Science
- Volume:
- 387
- Issue:
- 6733
- ISSN:
- 0036-8075
- Page Range / eLocation ID:
- eado7201
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract For advancing next‐generation optoelectronics, a versatile strategy for fabricating π‐conjugated polymer (π‐CP)/chiral‐small molecule (SM) hybrid films through co‐crystallization‐mediated chirality transfer is reported. The transfer of optical chirality from 1,1′‐binaphthyl–2,2′‐diamine (BN), a representative chiral inducer SM, to thin films of various achiral π‐CPs, including non‐fluorene π‐CPs, is achieved by simply blending the π‐CPs with BN using aromatic organic solvents. The resulting π‐CP/chiral‐SM hybrid films exhibit chiroptical responses at the main electronic absorption bands of various π‐CPs. Studies of the morphology, crystalline structure, and phase‐separation structure of a representative hybrid system of poly(3‐hexylthiophene) (P3HT) and BN reveal that these hybrid films exhibit a characteristic lamellar structure where the π‐CPs co‐crystallize with chiral BN molecules, facilitated by aromatic solvent‐assisted intermolecular π–π interactions. In‐depth photophysical analysis suggests that BN molecules co‐crystallized in the P3HT lamellar structure induce asymmetrically misaligned transition dipoles along the P3HT conjugated backbone, transferring optical chirality from BN to P3HT under circularly polarized light illumination. As a proof‐of‐concept, chiroptical photodiodes based on π‐CP/chiral‐SM hybrid films and printed micropatterns, exhibiting a distinguishable photocurrent response depending on the direction of circularly polarized light are successfully demonstrated.more » « less
-
Abstract Rational design of chiral two‐dimensional hybrid organic–inorganic perovskites is crucial to achieve chiroptoelecronic, spintronic, and ferroelectric applications. Here, an efficient way to manipulate the chiroptoelectronic activity of 2D lead iodide perovskites is reported by forming mixed chiral (R‐ or S‐methylbenzylammonium (R‐MBA+or S‐MBA+)) and achiral (n‐butylammonium (nBA+)) cations in the organic layer. The strongest and flipped circular dichroism signals are observed in (R/S‐MBA0.5nBA0.5)2PbI4films compared to (R/S‐MBA)2PbI4. Moreover, the (R/S‐MBA0.5nBA0.5)2PbI4films exhibit pseudo‐symmetric, unchanged circularly polarized photoluminescence peak as temperature increases. First‐principles calculations reveal that mixed chiral–achiral cations enhance the asymmetric hydrogen‐bonding interaction between the organic and inorganic layers, causing more structural distortion, thus, larger spin‐polarized band‐splitting than pure chiral cations. Temperature‐dependent powder X‐ray diffraction and pair distribution function structure studies show the compressed intralayer lattice with enlarged interlayer spacing and increased local ordering. Overall, this work demonstrates a new method to tune chiral and chiroptoelectronic properties and reveals their atomic scale structural origins.more » « less
-
Abstract Molecular profiles of mesenchymal stem cells (MSCs) are needed to standardize the composition and effectiveness of MSC therapeutics. This study employs RNA sequencing to identify genes to be used in concert with CD264 as a molecular profile of aging MSCs at a clinically relevant culture passage. CD264−and CD264+populations were isolated by fluorescence-activated cell sorting from passage 4 MSC cultures. CD264+MSCs exhibited an aging phenotype relative to their CD264−counterpart. Donor-matched CD264−/+mRNA samples from 5 donors were subjected to pair-ended, next-generation sequencing. An independent set of 5 donor MSCs was used to validate differential expression of select genes with quantitative reverse transcription PCR. Pairwise differential expression analysis identified 2,322 downregulated genes and 2,695 upregulated genes in CD264+MSCs relative to donor-matched CD264−MSCs with a Benjamini–Hochberg adjustedp-value (BHpadj) < 0.1. Nearly 25% of these genes were unique to CD264−/+MSCs and not differentially expressed at a significance level of BHpadj < 0.1 in previous RNA sequencing studies of early- vs. late-passage MSCs. Least Absolute Shrinkage and Selection Operator regression identified microtubule-associated protein 1A (MAP1A) and pituitary tumor-transforming gene 1 (PTTG1) as predictive genes of CD264+MSCs. CombinedMAP1AandPTTG1expression correctly classified CD264 status of MSC samples with an accuracy of 100%. Differential expression and predictive ability ofMAP1AandPTTG1compared favorably with that of existing senescence markers expressed in early passage CD264−/+MSCs. This study provides the first linkage ofMAP1Ato CD264, aging and senescence. Our findings have application as quality metrics to standardize the composition of MSC therapies and as molecular targets to slow/reverse cellular aging.more » « less
-
Abstract In this manuscript, we report the first demonstration of controlled helicity in extended graphene nanoribbons (GNRs). We present a wealth of new graphene nanoribbons that are a direct consequence of the high‐yielding and robust synthetic method revealed in this study. We created a series of defect‐free, ultralong, chiral cove‐edged graphene nanoribbons where helical twisting of the graphene nanoribbon backbone is tuned through functionalization with chiral side chains.S‐configured point chiral centers in the side chains transfer their chiral information to induce a helically chiral, right‐handed twist in the graphene nanoribbon. As the backbone is extended, these helically twisted graphene nanoribbons exhibit a substantial increase in their circular dichroic response. The longest variant synthesized consists of an average of 268 linearly fused rings, reaching 65 nm in average length with nearly 10 full end‐to‐end helical rotations. The structure exhibits an extraordinary |Δε| value of 6780 M−1cm−1at 550 nm—the highest recorded for an organic molecule in the visible wavelength range. This new chiroptic material acts as room‐temperature spin filters in thin films due to its chirality‐induced spin selectivity.more » « less
An official website of the United States government
