Mechanochemical engineering of chiroptical properties in indium-based chiral metal halides by grinding

Domain: physics
Published: 2026-02-11
Editorial outcome: minor_revision

Abstract
Circularly polarized luminescence is crucial for optoelectronics, bioimaging, and three-dimensional display, yet most of current materials suffer from complex synthesis and limited tunability. Herein, we show the regulation of chiroptical properties in metal halides through mechanochemical engineering. Specifically, phosphorescent indium-based chiral metal halides exhibit blue circularly polarized luminescence, along with antimony-doped indium-based metal halides emit orange circularly polarized luminescence. A grinding strategy using bromide salts like potassium bromide induces bright yellow fluorescence and enables versatile circularly polarized luminescence modulation. When antimony-doped indium-based metal halides are ground with five different bromide salts, it exhibits intriguing and tunable properties: (i) enhanced circularly polarized luminescence, with a luminescence dissymmetry factor value up to 10⁻²; (ii) inversion of the circularly polarized luminescence signal; (iii) generation of near-infrared circularly polarized luminescence with a substantial Stokes shift of 370 nm; and most notably, (iv) a 29.71-fold improvement in second-harmonic generation efficiency. This approach also realizes applications in circularly polarized light-emitting diodes.

Introduction
Materials with circularly polarized luminescence (CPL) activity have attracted extensive attention due to their potential applications in various fields such as three-dimensional (3D) optical displays, storage devices, molecular switches, optical sensors, information storage, and chiral sensing. The high-performance CPL materials require bright photoluminescence (PL), high photoluminescence quantum yield (PLQY) and a large luminescence dissymmetry factor (g_lum). Theoretically, achieving a high g_lum depends on the balanced contribution of the magnetic transition dipole moment and the electric transition dipole moment, in terms of both their magnitude and relative orientation. However, due to the intrinsic mismatch between magnetic and electric dipole transitions, simultaneously achieving high PLQY and g_lum remains a challenge. Chiral organic-inorganic metal halides have emerged as promising candidates for CPL materials owing to their tunable optoelectronic properties.

Current CPL regulation of chiral metal halides can be categorized into two approaches: crystal synthesis and post-regulation by external stimulation. The former approach predominantly relies on the selection of organic ligands and strategic metal doping during crystal growth. For instance, to obtain near-infrared (NIR) CPL, it is necessary to select the introduction of rare earth metals or iodide ions during the synthesis of the crystal. However, the growth of single crystals often requires a considerable time investment, and the quality of the crystals must be carefully monitored to obtain high-performance CPL metal halide materials. Recent studies have demonstrated post-synthetic CPL modulation through external stimuli, such as solvent treatment (e.g., dimethylformamide or acetonitrile), or high-pressure treatment. These approaches have laid the foundation for obtaining multi-colored, high-g_lum (>10⁻³) chiral metal halides. However, the current post-regulation methods for the CPL of metal halides are relatively limited with strict experimental conditions and complex synthetic processes, featuring high time costs and restricted CPL signal regulation. Therefore, it is urgent and necessary to develop simple and versatile ways to achieve effective and universal regulation of CPL properties for chiral metal halide materials.

In this work, we have developed a simple, rapid and generally applicable grinding strategy for post-regulation of chiral perovskites. First, chiral indium metal halides R/S-(1-amino-2-propanol)₂InCl₅ (denoted as R/S-In) were constructed through appropriate chiral selection ((R)-(-)-1-amino-2-propanol, (S)-(+)-1-amino-2-propanol), which show room-temperature phosphorescence (RTP) with long luminescence lifetimes of 96.74 and 86.34 ms, along with blue CPL emission. With the doping of Sb, R/S-InSb were obtained, which show orange symmetric CPL signals. Grinding R/S-InSb with a series of bromide salts enables tuning of the chiroptical and nonlinear optical properties. Both inorganic and organic salts can enhance the luminescence performance through grinding, thereby amplifying |g_lum| to the 10⁻² level. The selection of salts can also modulate the PL emission wavelength. After grinding R/S-InSb with FABr, the CPL signal in the visible light region red-shifts to the NIR region without adding any rare earth metals or introducing iodide ions. In addition to achieving multi-color CPL regulation, the grinding strategy can also reverse the CPL signal and enhance the second-harmonic generation (SHG) signal by 29.71-fold (Fig. 1a). Meanwhile, the grinding strategy endows the material with adjustable chiral optical properties, affording application potential in circularly polarized light-emitting diodes (CP-LEDs). In summary, this simple post-regulation strategy provides an approach for the preparation and application of high-performance chiral metal halides.

Results
Optical properties of chiral indium-based metal halide
The chiral indium-based metal halides R/S-In were synthesized via a hydrothermal method using chiral amino alcohol ligands ((R)-(-)-1-amino-2-propanol and (S)-(+)-1-amino-2-propanol). The phase purity and structural integrity were verified by powder X-ray diffraction (PXRD) analysis (Supplementary Fig. 1). Steady-state PL spectra reveal a primary emission band centered at 440 nm with a broad spectral profile spanning the 400-700 nm range, corresponding to sky-blue PL under UV excitation. Notably, persistent phosphorescence was directly observed in R/S-In samples after the cessation of UV irradiation. The phosphorescent nature of the emission was further verified by delayed PL spectra and time-resolved PL decay curves (Fig. 1b–e). The phosphorescence lifetime of R-In was tested as 96.74 ms, and that of S-In was tested as 86.34 ms. Further, the chiral optical properties of R/S-In were studied. As shown in Supplementary Fig. 2, there is a symmetrical circular dichroism (CD) signal in the 300-450 nm region of R/S-In, indicating that the chiral ligands have transferred chirality between the In-Cl octahedral structures. Additionally, in the 400-700 nm range, R-In shows a positive CPL signal, while S-In shows a negative CPL signal (Fig. 1f).

Element doping is an effective way to regulate the PL performance of metal halide. We introduced 15% Sb into R/S-In to red-shift the PL emission region of metal halides from blue to orange. The emission peak is located at 660 nm, presenting a wide and red-shifted emission peak, indicating that it belongs to the self-trapped state (STE) emission (Fig. 1b). The chiroptical properties of R/S-InSb were tested. The CD spectra revealed distinct mirror-image signals at 415 and 360 nm (Supplementary Fig. 4), indicating that the doping of Sb ions did not cause the disappearance of a chiral structure. As shown in Fig. 1c, the main diffraction peak of S-In and S-InSb is at 7.5°, which slightly shifts to a low angle with the doping of Sb³⁺, indicating that the doping of Sb³⁺ causes a slight lattice expansion, but it does not destroy the In-based crystal structure, and Sb³⁺ cations play a role by replacing In³⁺ cations into the crystal to form PL centers.

Modulation of PL by grinding
Grinding the sample with potassium bromide (KBr) and then pressing it into particles is a common sample preparation method, which is used to characterize its optical properties, including FTIR, UV-Vis, CD, CPL, PL, etc. Intriguingly, during our standard preparation of R/S-InSb with KBr, we discovered that the grinding process induced a dramatic color change of the photoluminescence to golden yellow (Supplementary Movie 1). In addition to KBr, various bromide salts including cesium bromide (CsBr), methylammonium bromide (MABr), guanidinium bromide (GuaBr), and formamidinium bromide (FABr) were found to react with R/S-InSb through mechanochemical grinding, yielding a series of composites (R/S-KBr, R/S-CsBr, R/S-MABr, R/S-GuaBr, and R/S-FABr). This outcome underscores the remarkable generality of the grinding strategy for post-synthetic modification.

Real-time photographic imaging of the ground crystals reveals emission wavelength shifts, prompting systematic photophysical characterization of the ground samples (Fig. 2a–f). Notably, S-KBr exhibits a 50 nm blue-shift relative to pristine S-InSb, with a dominant emission peak at 600 nm corresponding to bright yellow PL. The PLQY shows a 3.5-fold enhancement, reaching 35.51%. In contrast to KBr, grinding R/S-InSb with the other four bromide salts resulted in a distinct red shift in the PL spectra of the resulting composites (R/S-CsBr, R/S-MABr, R/S-GuaBr, and R/S-FABr). It is worth noting that, the emission peak position of S-FABr red shifts to 735 nm, with the Stokes shift as large as 370 nm (Fig. 2c). The emission peak extends from 550 to 1200 nm, achieving a wide spectral coverage in the NIR region. Generally speaking, to achieve NIR emission from metal halides, rare earth metal ions need to be introduced or halide ions need to be replaced with I⁻ anions. Remarkably, the metal halides in this work realize NIR emission via a straightforward grinding strategy, without incorporating any rare-earth metals or additional foreign elements. As shown in Fig. 2d, the absorption of the crystals after grinding shifted towards the red compared to the crystals before grinding, which indicates that the Br⁻ ions have been incorporated into the system. To further investigate the existence form of Br⁻ in the system, we conducted energy dispersive spectroscopy (EDS) mapping on the ground sample after grinding (Supplementary Fig. 5). The EDS mapping results revealed the overlap between the Br⁻ and Cl⁻ signals in the transmission electron microscopy images, indicating a highly homogeneous distribution of Br elements throughout the observed regions, closely coinciding with the Cl distribution. This provides evidence that Br⁻ has been uniformly doped into the bulk phase of the material. Quantitative analysis of the Br signal relative to the total halogen signal (Br⁻ + Cl⁻) further indicated an influence of the cation species on the bromine substitution process. Specifically, inorganic bromide salts generally resulted in a lower relative atomic percentage of Br compared to organic bromide salts. Notably, the S-KBr sample exhibited the lowest Br relative percentage of merely 12.72%. In contrast, among the organic bromide salts, the S-MABr sample achieved the highest Br relative atomic percentage of 93.48%. To further elucidate the existence form of Br⁻, X-ray photoelectron spectroscopy (XPS) analysis was conducted on all ground samples (Supplementary Figs. 6–10). The relative atomic percentages of Br obtained from XPS showed a trend similar to that derived from EDS analysis (Supplementary Table 7). A notable discrepancy was observed for the S-KBr sample, where the Br percentage differed between EDS (bulk-sensitive) and XPS (surface-sensitive) measurements. This suggests a lower efficiency of bromine substitution in S-KBr, with Br⁻ predominantly located near the sample surface. Conversely, for the S-CsBr, S-MABr, S-FABr, and S-GuaBr samples, the consistent Br percentages from both XPS and EDS mapping indicate a more substantial incorporation of Br⁻ into the bulk phase.

To thoroughly investigate the universality of our grinding strategy and elucidate the critical role of halide anions, we extended our research to include chloride and iodide salt systems. As shown in Supplementary Fig. 11, the choice of halide anion proved decisive for the optical modulation outcome: most chloride salts (e.g., KCl, CsCl, MACl, GuaCl) induced a blue shift in the photoluminescence spectrum. Although both formamidinium chloride (FACl) and FABr caused a red shift, the magnitude of the shift induced by FABr was greater than that by FACl. Most notably, all iodide salts led to complete fluorescence quenching. These results reveal a synergistic cation-anion mechanism during the grinding process: the nature of the cation primarily governs the direction of the spectral shift, while the properties of the halide anion (particularly its ionic size) dictate the extent and ultimate success of the spectral modulation. This underscores that careful consideration of the size compatibility between the cationic and anionic constituents of the grinding salt is crucial for achieving efficient optical modulation.

Amplification and inversion of CPL by grinding
To investigate the grinding-induced changes in chiral optical properties, we systematically characterized the CD spectra and powder X-ray diffraction (PXRD) patterns of ground samples. Although modified substances were generated after the mechanical chemical treatment, they still maintained the chiral properties and crystal characteristics (Supplementary Figs. 12–22). Corresponding circularly polarized luminescence (CPL) measurements revealed mirror-symmetric signals for the parent R/S-InSb within the 500–800 nm range (Fig. 3a), with R-InSb exhibiting a positive signal and S-InSb showing a negative signal. The g_lum value calculated from the CPL signals is approximately ±1 × 10⁻³. We further evaluated the CPL properties of the ground composites—R/S-KBr, R/S-CsBr, R/S-MABr, R/S-GuaBr, and R/S-FABr—as summarized in Fig. 3b–f. Notably, R/S-KBr exhibited a 6-fold enhancement in CPL signal intensity compared to pristine R/S-InSb, with maximum |g_lum| values reaching 1 × 10⁻² (Supplementary Fig. 24). This indicates that KBr grinding amplifies the CPL dissymmetry factor by an order of magnitude to the 10⁻² level. This may be due to the fact that the inorganic cation K⁺ salt and anion Br⁻ greatly improves its emission performance, as confirmed by the PLQY characterization (Supplementary Table 8). The PLQY of S-InSb before grinding was 10.46%, and that of S-KBr was ≈3.5 times (35.51%) higher than before grinding. Similarly, S-CsBr also increased the PLQY by a factor of 2 (20.13%), resulting in an increase in the |g_lum| to 4 × 10⁻³ (Supplementary Fig. 25).

Mechanochemical grinding of R/S-InSb with organic salts also enabled CPL signal amplification, demonstrating the general applicability of this strategy. The introduction of FABr caused the main emission peak position to shift from 660 to 735 nm. The CPL spectrum shows a corresponding trend, presenting NIR CPL emission. R-FABr shows a positive signal CPL in the 500–900 nm region, while S-FABr shows a negative signal CPL in the same region. The direction of the CPL signal is consistent with that of R/S-InSb (Fig. 3f). To further explore the near-infrared emission mechanism of R/S-FABr, the temperature-dependent PL spectra of S-FABr were acquired. Supplementary Fig. 30 reveals simultaneous thermal quenching and spectral broadening, the full width at half maximum (FWHM) increases from 165 to 194 nm as temperature rises from 260 to 340 K. This combination of phenomena aligns with characteristic signatures of self-trapped exciton (STE) emission. Quantitative analysis of electron-phonon coupling strength yields a Huang-Rhys factor S=30.25, exceeding the strong-coupling threshold (S>5). This confirms substantial electron-phonon interaction in the material. Meanwhile, the exciton binding energy extracted from Arrhenius fitting (E_a = 138.50 meV) ensures adequate stability of the self-trapped state at room temperature. It is noteworthy that the samples ground with MABr not only amplified the original CPL signal but also reversed the direction of the CPL signal. Among them, R-MABr shows a negative CPL signal, which is opposite to the CPL signal direction of R-InSb, and their enantiomers also show similar trends. Compared with the ground samples with inorganic salts (R/S-KBr and R/S-CsBr), the PLQY of the ground samples with organic salts (MABr, GuaBr and FABr) showed no improvement (Supplementary Table 8). Therefore, the grinding of organic salts for achieving chiral amplification may be related to the formation of more tightly bound hydrogen bonds with small-sized cations, which affects the chiral transfer process, which has been confirmed by Raman spectroscopy. Compared with the Raman spectra of S-InSb before grinding, the methylene stretching vibration band at 2915 cm⁻¹ in S-MABr and S-GuaBr transformed from a single peak to a double peak after grinding (Supplementary Fig. 31). It indicates that the environment of the methylene group has changed due to the introduction of organic bromide salt. In the GuaBr grinding system, the characteristic sharp peak of pure GuaBr observed at 3317 cm⁻¹ undergoes a distinct shift to a higher wavenumber region (3328 cm⁻¹) upon grinding, accompanied by noticeable peak broadening. This observation indicates that the Gua⁺ cation plays a dual role in the grinding sample: it acts not only as a hydrogen bond donor but also contributes to the reconstruction and enhancement of the hydrogen bonding network (Supplementary Fig. 32). This resulted in an increase in the g_lum value of R/S-GuaBr, which was calculated as 1.34 × 10⁻² and −1.45 × 10⁻², respectively. The 3289–3558 cm⁻¹ region of S-MABr exhibited a broad envelope, indicative of dynamic reorganization in the hydrogen-bonding network. This structural reconfiguration is hypothesized to underpin the observed CPL signal inversion (Supplementary Fig. 33).

To elucidate the mechanism underlying CPL signal inversion, we obtained single-crystal structures of R/S-InSb and R/S-MABr via a slow-cooling crystallization method. Both compounds crystallize in the triclinic space group P1. In the crystal structure of S-InSb, the chiral structure is composed of In-Cl octahedra and chiral ligands. The chiral (R/S)-1-amino-2-propanol ligands were connected to the In³⁺ octahedra through three distinct hydrogen bonds. The hydroxyl group of the chiral ligand formed O-H···Cl hydrogen bonds with the Cl⁻ anion on the In³⁺ octahedron, with bond lengths ranging from 3.071 to 3.166 Å. The amino hydrogen formed longer N-H···Cl hydrogen bonds with the Cl⁻ anion on the octahedron (Fig. 4a and Supplementary Fig. 34). These hydrogen-bonding interactions collectively assemble into the crystal architecture depicted in Fig. 4b. Surprisingly, in the S-MABr crystal structure, we observed that methylamine molecules were not incorporated into the lattice. Instead, Br⁻ anions substituted for Cl⁻ anions on the In³⁺ octahedral after grinding. Notably, the hydrogen-bonding network in S-MABr exhibited greater complexity compared to S-InSb. In contrast to S-InSb where the chiral ligand exhibited three distinct hydrogen-bonding modes, (S)-(+)-1-amino-2-propanol in S-MABr exclusively forms N-H···Br hydrogen bonds with the octahedral Br⁻ anions, with bond lengths ranging from 3.383 to 3.398 Å (Fig. 4c and Supplementary Fig. 35). Additionally, a different O-H···O hydrogen bond (2.825 Å) emerged between two antiparallel chiral ligands. These hydrogen-bonding interactions collectively induce a more compact octahedral arrangement in S-MABr, enhancing CPL performance. Furthermore, by comparing the Raman spectra of S-MABr with those of other ground samples, we discovered that the hydrogen bond form of S-MABr, which is consistent with the phenomenon mentioned earlier where the CPL signals of only R/S-MABr in the CPL spectrum reversed (Supplementary Fig. 36). Critically, the octahedral packing in S-MABr adopted a chiral arrangement opposite to that in S-InSb. This reversed octahedral organization post-grinding directly underpinned the observed CPL signal inversion. The newly formed hydrogen bonds during grinding play a pivotal role in driving the structural reversal.

Enhancement of SHG by grinding
The ground samples still exhibited symmetric CD signals, confirming non-centrosymmetry and SHG potential. To verify this hypothesis, we tested the SHG properties of the samples before and after grinding, excited by a 1 W 860 nm laser (Fig. 5a). The results demonstrated a universal enhancement in SHG intensity for all ground samples (KBr, CsBr, MABr, GuaBr, FABr) compared to the pristine S-InSb (Supplementary Table 9). Among them, S-MABr shows the most improvement, with an enhancement of 5.18 times compared to S-InSb and 29.71 times compared to the standard sample Y-cut quartz. These results further demonstrate the effectiveness of the grinding process in regulating the chiral optical properties. The nonlinear optics (NLO) properties of S-MABr were further studied. The SHG spectrum obtained under femtosecond laser excitation from 800 to 900 nm revealed efficient second-harmonic conversion (Fig. 5b). Moreover, the power-dependent SHG intensity curve shows that the SHG intensity increases quadratically with the input laser power (Supplementary Fig. 37). This quadratic increase in SHG intensity confirms the second-order nonlinear optical process (Fig. 5c). To elucidate the structural origin of the SHG enhancement, we quantified the distortion of the metal-halide octahedra in R/S-InSb and R/S-MABr (Fig. 5d). The off-centering distortion index (D) and bond angle variance (σ²) are commonly used to quantify the asymmetry of the octahedra. The D and σ² are calculated using Eqs. (1) and (2) according to the refs. 56, 57. The D index of [InCl₆]³⁻ and [InBr₆]³⁻ are 0.018 and 0.030, respectively. The σ² values of [InCl₆]³⁻ and [InBr₆]³⁻ are 3.9605 and 5.9726, respectively. This clear increase in both distortion parameters indicates that Br⁻ substitution induces greater octahedral distortion compared to Cl⁻, which is the fundamental reason for the enhanced SHG response observed in S-MABr.

Grinding mechanism
The crystalline architecture of R/S-InSb affords a distinctive capacity for mechano-responsive optical modulation via grinding. Firstly, the chiral ligand R/S-1-amino-2-propanol, classified as the alcohol amine category, contains hydroxyl groups. Due to the electronegativity of oxygen, the hydrogen on the hydroxyl group is more prone to dissociation compared to the hydrogen on the amino group in most of the amine ligands reported in ref. 60. This inherent characteristic facilitates the formation of dynamic hydrogen-bonding networks within the metal-halide framework, thereby promoting solid-state reactivity during grinding. Secondly, comparative analysis with reported InSb-based chiral metal halides reveals that the alkanolamine-ligated metal halide exhibits a lower octahedral distortion index. This suggests that the hydrogen-bonding interactions between the chiral ligand and the [InCl₆]³⁻ octahedra are comparatively weaker than those in structures ligated by aliphatic or aromatic amines. Such structural characteristics provide a mechanistic basis for the occurrence of grinding-induced solid-state reactions.

Substantial structural reorganization is corroborated by unit cell parameter analysis. The parameters for S-InSb (α=84.790°, β=84.016°, γ=64.131°) shift upon grinding with MABr, yielding S-MABr with parameters α=68.381°, β=75.213°, γ=71.843°. This pronounced change unequivocally indicates a major crystal phase transition. To gain deeper insight into the grinding-induced reaction, we performed density functional theory (DFT) calculations to simulate the interaction between S-InSb and MABr. The computed reaction enthalpy is ΔH=–17.03 kJ mol⁻¹ (Fig. 5e), suggesting an exothermic process. It is thus plausible that a fraction of the mechanical energy input during grinding is converted into localized heat, elevating the temperature at the interface and driving the chemical transformation. Consequently, the crystal undergoes a phase transition from S-InSb to S-MABr, a process that entails reversal of the octahedral arrangement direction, adoption of a more compact structural packing, and halogen substitution.

Application in CP-LEDs
Owing to the grinding strategy that confers samples with wavelength-tunable luminescence performance and CPL characteristics, the samples were pasted on a commercial GaN ultraviolet light-emitting diode (UV-LED) chip (365 nm, 1.0 W) to get the CP-LED device at the 5 V driving voltage, the CPL properties of the UV-LED devices were characterized (Fig. 6a–f). It is worth noting that a series of CP-LED devices exhibit mirror-symmetric CPL signals within the range of 500–900 nm, with the position of the main emission peak wavelength and the circularly polarized direction being highly consistent with the previously measured CPL spectra. Notably, the CP-LED devices fabricated with the R-GuaBr and S-GuaBr samples exhibited the maximum |g_lum| values of ≈+1.37 × 10⁻² and −1.98 × 10⁻², respectively (Supplementary Fig. 38). This indicates that the materials obtained through the grinding strategy have great application potential for CP-LED devices.

Methods
Materials
Indium(Ⅲ) chloride (InCl₃), (R)-1-amino-2-propanol, (S)-1-amino-2-propanol, N,N-dimethylformamide (DMF) were purchased from Heowns. Antimony trichloride (SbCl₃) was purchased from Meryer. Potassium bromide (KBr), cesium bromide (CsBr), methylamine bromide (MABr), guanidinium bromide (GuaBr), and formamidine bromide (FABr) was purchased from Macklin. Hydrochloric acid (36–38%) was purchased from Tianjin Fengchuan chemical company.

Synthesis of R-/S-1-amino-2-propanol hydrochloride. R-/S-1-amino-2-propanol (0.05 mol) was added to absolute ethanol (20 mL) and dissolved into a pellucid yellow transparent solution under stirring at room temperature. Then, hydrochloric acid (36–38%, 10 mL) was dripped into the reaction system with a dropping funnel at a uniform speed, and the reaction continued for 4 h until white powder was gradually precipitated. After the reaction, absolute ether was added for washing, filtering and repeating three times to obtain white powder. Finally, the product was dried in a vacuum drying oven at 50 °C for 6 h to obtain R-/S-1-amino-2-propanol hydrochloride.

Synthesis of R/S-In crystals. InCl₃ (1 mmol, 221.4 mg) and R-/S-1-amino-2-propanol hydrochloride (2 mmol, 222.2 mg) was added to hydrochloric acid (36–38%, 2 mL) to react at 90 °C until the solid was completely dissolved, and the reaction continued for 2 h. After the reaction, the reaction solution was naturally cooled to room temperature, resulting in crystals to grow. Finally, R/S-In crystals were obtained by filtering, washing and drying.

Synthesis of Sb³⁺-doped R/S-InSb single crystals. 15% of InCl₃ in the precursor is replaced by SbCl₃, and the total molar amount remains unchanged. The synthesis of R/S-InSb single crystals is as follows. InCl₃ (0.85 mmol, 187.2 mg), SbCl₃ (0.15 mmol, 34.8 mg) and R-/S-1-amino-2-propanol hydrochloride (2 mmol, 222.2 mg) was added to hydrochloric acid (36–38%, 2 mL) to react at 90 °C until the solid was completely dissolved, and the reaction continued for 2 h. Subsequent steps remain the same with that of R/S-In. Finally, R/S-InSb single crystals were obtained by filtering, washing and drying.

Synthesis of Sb³⁺-doped R/S-MABr single crystals. The synthesis of R/S-MABr single crystals is as follows. InCl₃ (0.85 mmol, 187.2 mg), SbCl₃ (0.15 mmol, 34.8 mg), R-/S-1-amino-2-propanol hydrochloride (2 mmol, 222.2 mg) and methylammonium bromide (2 mmol, 223.94 mg) was added to hydrochloric acid (36–38%, 2 mL) to react at 90 °C until the solid was completely dissolved, and the reaction continued for 2 h. Subsequent steps remain the same with that of R/S-In. Finally, R/S-InSb single crystals were obtained by filtering, washing and drying.

Sample preparation for CPL/CD measurements. The powder was dissolved anhydrous DMF under mild stirring to form a clear, homogeneous solution. The solution was then spin-coated onto meticulously cleaned quartz substrates. The spin-coating parameters were rigorously controlled: a speed of 2000 revolutions per minute (rpm) for a duration of 30 s. Immediately after spin-coating, the films were transferred to a hot plate and annealed at 100 °C for 10 min.

Characterization
A LAMBDA 750 ultraviolet spectrometer was used to measure the UV-visible absorption spectrum of solids. PL spectrum, PLE spectrum, delayed PL spectrum and PLQY were measured at Edinburgh FLS1000 under excitation at 365 nm.

Single crystals of R/S-InSb were recorded using the Bruker D8 Venture TXS PHOTON 100 diffractometer. The crystal was kept at 100 K during data collection. Using Olex2, the structure was solved with the SHELXT structure solution program using Intrinsic Phasing and refined with the SHELXL refinement package using Least Squares minimization.

The crystal structure of chiral In-based metal halide powders has been characterized by an X-ray diffractometer with Cu Kα radiation (λ=1.5418 Å). The measurement range is 5−90° and the scanning speed is 10° min⁻¹.

The X-ray photoelectron spectroscopy (XPS) measurements were performed with a ThermoFisher Scientific ESCALAB 250Xi spectrometer using a monochromatic Al Kα source (1486.6 eV). All spectra were charge-corrected to the C 1s peak at 284.8 eV.

TEM images and elemental distributions of the samples were collected on a field-emission transmission electron microscope JEM-F200.

The CD spectra was tested at room temperature with JASCO-J1700 CD spectrometer (scan speed 500 nm min⁻¹ (digital integration time (DIT): 1 s).

CPL was tested with the circularly polarized PL spectrometer of CPL-300 (scan speed 500 nm min⁻¹, DIT: 1 s).

The SHG spectra was measured with a WITec alpha 300R.

The LED device is made by mixing grinding samples with PDMS and then coating it on the commercialized UV-LED chips. Excitation is carried out with the current of 5 V 0.2 A.

All the calculations are implemented by the VASP code. The GGA-PBE functional is selected for the exchange and correlation potential. Weak van der Waals interaction is considered by the DFT-D3 functional. The cut-off energy for the plane-wave is 400 eV. The Gamma point in the Brillouin-zone is chosen for integration. Total energies of the systems converge to 10⁻⁵ eV in the iteration solution of Kohn-Sham equation. The force on each atom reduces to 0.05 eV Å⁻¹ after geometry optimization.

Peer review rounds
[{"round": 1, "reviewer_comments": {"reviewer_1": "The authors report the first phosphorescent indium-based chiral metal halides with blue CPL emission. It is interesting that the grinding process of R/S-InSb enable amplification, inversion, and near-infrared modulation of CPL signals, demonstrating high novelty. The grinding strategy completes solid-phase reactions within 10 seconds and works for various organic/inorganic bromide salts, significantly enhancing the CPL dissymmetry factor (|gₗᵤₘ| up to 10⁻²) and enabling signal inversion. This provides an efficient and universal approach for chiral optical modulation. Therefore, it is suggested that the paper be accepted after minor revisions and published in Nature Communications.\n1. The paper mentions the glum values of the materials before and after grinding, but the glum value of the indium-based metal halides (R/S-In) is not mentioned. This experimental data needs to be supplemented and provided either in the main text or in the supplementary materials.\n2. In the section on enhancing the grinding strategy for metal halide perovskite CPL, no textual description was provided on how GuaBr enhances CPL and the glum value. It is recommended to include this information in the main text to highlight the advantages of enhancing the chiral optical properties.\n3. The article describes the interesting phenomenon of optical control achieved through the grinding of R/S-InSb with bromide salts. It suggests trying some new salts, such as whether chloride salts have a similar phenomenon to bromide salts, in order to enrich the universality of the strategy.\n4. The article mentions instruments such as the CPL-300 and CD-J1700, but the details of the tests are not described adequately. The scanning speed and D.I.T in the CD and CPL measurements should be provided.\n5. The illustrations in the article are very aesthetically pleasing, but some of the annotations within the figures need to be aligned with the text and have a uniform font size. For instance, the text parts in Figure 3 and Figure 5c could be appropriately modified.", "reviewer_2": "This paper reports a mechanochemically induced post-regulation strategy for tuning the chiroptical properties of indium-based metal halides through a “Midas touch”-inspired grinding process. By introducing various bromide salts during the grinding treatment, the authors demonstrate remarkable modulation of circularly polarized luminescence (CPL), including the amplification of glum, CPL signal inversion, near-infrared (NIR) emission with a large Stokes shift, and a enhancement of second-harmonic generation (SHG) response. Moreover, the authors illustrate potential device-level applications such as CP-LEDs, optical logic gates, and anti-counterfeiting displays. The reviewer thinks that researchers in this field will be interested in the results of this manuscript. However, there are some issues needed to be clarified by the authors before publication as below. The following comments are not to criticize but to strengthen the manuscript.\n1. The authors suggest that Br– are incorporated into the crystal lattice during the grinding process, but the current data (PXRD, Raman) do not provide conclusive proof. Additional evidence such as XPS spectra, EDS mapping, or refined single-crystal XRD data would be necessary to confirm whether Br– truly substitutes Cl– or is only adsorbed on the surface.\n2. The authors state that the ground samples form new crystalline phases, yet the manuscript does not provide any data on their long-term or environmental stability. Since these materials are proposed for optoelectronic applications, the authors should clarify whether the CPL intensity, PLQY, and SHG efficiency remain stable under ambient conditions (air, humidity, light exposure) or degrade over time.\n3. In Figure 1c, the presented XRD pattern seems to correspond to InSb, but the discussion in line 76 mainly focuses on the phosphorescent properties of R/S-In. It would be helpful if the authors could clearly indicate in the figure caption or text which sample the XRD data represent, to avoid possible confusion.\n4. In the main text (lines 79-80), Figure S2 is described as showing the CD spectrum of R/S-In, whereas the actual Figure S2 in the supplementary information appears to present the CD spectrum of InSb. The figure and the text should be aligned.\n5. Due to the missing Figure S2 (In CD spectrum), all subsequent supplementary figures seem to have been shifted by one position (e.g., what is labeled as S3 should actually be S2). The figure numbering in the supplementary section should be carefully checked and corrected.\n6. In line 98, the text refers to “Fig. 1b,” but it should correspond to “Fig. 1c.” The figure citation should be corrected.\n7. In Figure S12, the sample is labeled as “MA,” although it represents MABr. The notation should be corrected to “MABr” for consistency with the figure caption and the main text.\n8. The authors suggest that stronger hydrogen bonding with small cations (e.g., Gua+) enhances chiral transfer. However, the manuscript does not provide experimental evidence verifying the stronger hydrogen bonding in GuaBr. It is more likely that Gua+ introduces additional NH donors rather than intrinsically stronger H-bonds. Comparison with pure GuaBr and pure MABr samples would clarify whether the observed effects result from hydrogen-bond network reconstruction or simply from the presence of organic bromide species.\n9. In lines 182–184, Cl– is introduced without prior explanation. The authors should clarify earlier that the pristine material (InSb) is composed of In–Cl octahedra and specify the origin of Cl– before discussing Br⁻ substitution.\n10. The authors state that in S-MABr, MA+ does not enter the lattice and that Cl– is replaced by Br– after grinding, forming N–H···Br hydrogen bonds. If the newly formed hydrogen bonds are indeed responsible for the opposite chiral arrangement, it should be clarified whether such Br– substitution also occurs in the other bromide salts (KBr, CsBr, GuaBr, FABr), or if Cl– remains in those cases. This point is crucial, as the enhanced SHG response is also explained by Br– substitution.\n11. In line 270, the manuscript reports maximum glum values of approximately 1.37 × 10–2 and -1.98 × 10–2, but it is unclear from which sample these values were obtained. The authors should specify the measurement source and include the corresponding CPL (glum) spectra in the Supporting Information for clarity.\n12. As the samples are powder forms of single crystal, it is difficult to measure CPL and CD of these samples. Please explain how the authors made samples and took measurements?\n13. In CP-LED applications, are all UV excitation light absorbed by singe crystals? If not, there should be some leakage lights which are not absorbed by the single crystals.", "reviewer_3": "This manuscript presents a highly innovative and significant study on the post-synthetic regulation of chiral indium-based metal halides using a simple grinding strategy. The \"Midas touch\" approach demonstrates remarkable versatility, enabling multifaceted modulation of key optical properties—including CPL amplification, inversion, NIR emission, and a dramatic enhancement of SHG. The work showcases compelling applications in CP-LEDs, logic gates, and anti-counterfeiting. Generally speaking, this work is meticulously executed, and the findings are of significant interest. It may worth the attention of the readership of Nature Communications if the following points are appropriately addressed.\n1. Is the effect unique to bromide salts? Control experiments with chloride or iodide salts (e.g., KCl) would be highly informative to delineate whether anion exchange (Cl⁻ to Br⁻) is the primary driver or if cations and mechanical force play more complex roles. This is crucial, as halogen substitution has been shown to significantly alter optical properties in chiral metal halides.\n2. The achievement of NIR CPL without rare-earth metals or I⁻ ions is significant. It is better to expand the discussion on how the grinding with FABr specifically modifies the STE states or band structure to enable such a large Stokes shift and NIR emission, potentially referencing relevant studies on STE emission in metal halides.\n3. In Figure 3b, d, e, the CPL spectra of the ground samples (e.g., R/S-KBr, R/S-GuaBr, R/S-MABr) are not perfectly symmetrical. This asymmetry may indicate a change in the emission mechanism or the presence of multiple emitting species with different chiral environments. Please provide the corresponding total fluorescence (DC) spectra and give a plausible explanation for this phenomenon.\n4. Several figures in SI are cited incorrectly. Please review them to ensure accurate citations throughout the manuscript.\n5. Some recently published related papers may be of reference value, e.g., 10.1021/acs.accounts.3c00599, 10.1002/anie.202308194.\n6. The manuscript contains a few typographical errors, grammatical mistakes, and occasionally awkward phrasing that detract from the scientific narrative. To meet the high publication standard, a comprehensive line-by-line revision is recommended of the entire manuscript."}, "author_response": "Responses to Reviewers’ Comments\nReviewer #1 (Remarks to the Author):\nThe authors report the first phosphorescent indium-based chiral metal halides with blue\nCPL emission. It is interesting that the grinding process of R/S-InSb enable\namplification, inversion, and near-infrared modulation of CPL signals, demonstrating\nhigh novelty. The grinding strategy completes solid-phase reactions within 10 seconds\nand works for various organic/inorganic bromide salts, significantly enhancing the CPL\ndissymmetry factor (|gₗᵤₘ| up to 10⁻²) and enabling signal inversion. This provides an\nefficient and universal approach for chiral optical modulation. Therefore, it is suggested\nthat the paper be accepted after minor revisions and published in Nature\nCommunications.\nComment 1-1. The paper mentions the g values of the materials before and after\nlum\ngrinding, but the g value of the indium-based metal halides (R/S-In) is not mentioned.\nlum\nThis experimental data needs to be supplemented and provided either in the main text\nor in the supplementary materials.\nResponse 1-1: We sincerely thank the reviewers for prompting us to provide additional\nexplanations of the data. In response to your comments, we have added in the\nsupporting information section of the paper the values of the luminescence asymmetry\nfactor (g ) for the indium-based metal halides discussed in this study.\nlum\nFig. R1-1 The g factor of R/S-In.\nlum\nComment 1-2. In the section on enhancing the grinding strategy for metal halide\nperovskite CPL, no textual description was provided on how GuaBr enhances CPL and\nthe g value. It is recommended to include this information in the main text to\nlum\nhighlight the advantages of enhancing the chiral optical properties.\nResponse 1-2: We are grateful for the constructive suggestions provided by the\nreviewers. Through the Raman spectra of S-GuaBr, GuaBr, and S-InSb samples, the\ncharacteristic sharp peak of pure GuaBr observed at 3317 cm⁻¹ undergoes a distinct\nshift to a higher wavenumber region (3328 cm⁻¹) upon grinding, accompanied by\nnoticeable peak broadening (Fig. R1-2). Therefore, GuaBr has enlarged the hydrogen\nbond network of the system by providing more hydrogen bond sites, and we have\nsupplemented this description as well as the g lum value of R/S-GuaBr (1.34 × 10-2 and -\n1.45 × 10-2) into the main text, which is very helpful for highlighting the performance\nadvantages of the material.\nFig. R1-2 The Raman spectra of S-InSb, GuaBr and S-GuaBr.\nComment 1-3. The article describes the interesting phenomenon of optical control\nachieved through the grinding of R/S-InSb with bromide salts. It suggests trying some\nnew salts, such as whether chloride salts have a similar phenomenon to bromide\nsalts, in order to enrich the universality of the strategy.\nResponse 1-3: Thanks for the reviewer for the very helpful suggestions. Our control\nexperiments reveal that the effect works for both bromide salts and chloride salts, but\nbromide salts consistently induce the most pronounced changes. The results highlight\na complex interplay between the halide anion (X⁻) and the cation (A⁺) during the\nmechanochemical process.\nChloride and Bromide Salts Induce Cation-Dependent Spectral Shifts: More\nimportantly, grinding with chloride salts (Fig. R1-3a) also induces significant shifts in\nthe PL spectrum compared to pristine S-InSb, confirming that anion exchange (Cl⁻ for\nCl⁻/Br⁻) is not the sole driver. The direction and magnitude of the shift (blue or red) are\nstrongly influenced by the cation: For salts with the same cation, Br⁻ substitution\nconsistently induces a larger spectral shift than Cl⁻ substitution (S-FABr vs. S-FACl)\n(Fig. R1-3c-h). This demonstrates that Br⁻ is more effective in modulating the electronic\nstructure (e.g., band gap or STE energy level), likely due to its appropriate ionic radius\nand electronegativity.\nIodide Salts Cause PL Quenching: As shown in Fig. R1-3b, grinding S-InSb with any\nof the iodide salts (e.g., CsI, MAI, FAI, GuaI) results in complete or near-complete\nquenching of the PL signal. This suggests that the large ionic radius of I⁻ disrupts the\noriginal crystal structure of S-InSb during grinding, preventing the formation of a stable,\nluminescent phase. This observation underscores that successful modification requires\ncompatible halide ionic radii.\nThe corresponding figures and discussions are supplemented into the manuscript and\nSI.\nFig. R1-3 a PL photos of the S-InSb and the samples after grinding treatment wih\nchloride and b iodate salts under 365nm ultraviolet light irradiation. c-h The PL\nspectra of S-InSb, S-KBr, S-KCl, S -CsBr, S-CsCl, S -MABr, S-MACl, S-GuaBr, S-\nGuaCl, S-FABr and S-FACl.\nComment 1-4. The article mentions instruments such as the CPL-300 and CD-J1700,\nbut the details of the tests are not described adequately. The scanning speed and D.I.T\nin the CD and CPL measurements should be provided.\nResponse 1-4: We thank the reviewer for the attention to instrumental details. As\nsuggested, we have supplemented the materials characterization section in the\nmanuscript with the following key parameters for Circular Dichroism (CD) and\nCircularly Polarized Luminescence (CPL) measurements:\nCD parameters: Scan speed 500 nm/min, D.I.T: 1 s\nCPL parameters: Scan speed 500 nm/min, D.I.T: 1 s\nComment 1-5. The illustrations in the article are very aesthetically pleasing, but some\nof the annotations within the figures need to be aligned with the text and have a uniform\nfont size. For instance, the text parts in Figure 3 and Figure 5c could be appropriately\nmodified.\nResponse 1-5: We are grateful to the reviewers for pointing out the issue of the neatness\nof the annotations in the figures. During the revision of the manuscript, we carefully\nchecked all the annotations of the figures and corrected corresponding figures to\nmaintain the readability and aesthetics of the manuscript.\nReviewer #2 (Remarks to the Author):\nThis paper reports a mechanochemically induced post-regulation strategy for tuning the\nchiroptical properties of indium-based metal halides through a “Midas touch”-inspired\ngrinding process. By introducing various bromide salts during the grinding treatment,\nthe authors demonstrate remarkable modulation of circularly polarized luminescence\n(CPL), including the amplification of g , CPL signal inversion, near-infrared (NIR)\nlum\nemission with a large Stokes shift, and an enhancement of second-harmonic generation\n(SHG) response. Moreover, the authors illustrate potential device-level applications\nsuch as CP-LEDs, optical logic gates, and anti-counterfeiting displays. The reviewer\nthinks that researchers in this field will be interested in the results of this manuscript.\nHowever, there are some issues needed to be clarified by the authors before publication\nas below. The following comments are not to criticize but to strengthen the manuscript.\nComment 2-1. The authors suggest that Br– are incorporated into the crystal lattice\nduring the grinding process, but the current data (PXRD, Raman) do not provide\nconclusive proof. Additional evidence such as XPS spectra, EDS mapping, or refined\nsingle-crystal XRD data would be necessary to confirm whether Br– truly substitutes\nCl– or is only adsorbed on the surface.\nResponse 2-1: We sincerely thank the reviewer for the constructive suggestions\nprovided for our manuscript. To further investigate the chemical state and distribution\nof bromide ions (Br⁻) in the post-grinding samples, we performed comprehensive\ncharacterization using energy dispersive spectroscopy (EDS) and x-ray photoelectron\nspectroscopy (XPS).\nThe EDS mapping results revealed a near-perfect overlap between the Br⁻ and Cl⁻\nsignals in the transmission electron microscopy images, indicating a highly\nhomogeneous distribution of Br elements throughout the observed regions, closely\ncoinciding with the Cl distribution (Fig. R2-1). This provides strong evidence that Br-\nhas been successfully and uniformly doped into the bulk phase of the material.\nQuantitative analysis of the Br signal relative to the total halogen signal (Br⁻ + Cl⁻)\nfurther indicated a significant influence of the cation species on the bromine\nsubstitution process. Specifically, inorganic bromide salts generally resulted in a lower\nrelative atomic percentage of Br compared to organic bromide salts. Notably, the S-\nKBr sample exhibited the lowest Br relative percentage of merely 12.72%. In contrast,\namong the organic bromide salts, the S-MABr sample achieved the highest Br relative\natomic percentage of 93.48%, a finding consistent with the single-crystal structure\nresolved in our manuscript (Table R2-1).\nFig. R2-1 The TEM image of S-KBr, S-CsBr, S-MABr, S-FABr, S-GuaBr and EDS\nmapping images of Cl (green), Br (purple) distributions.\nTo further elucidate the existence form of Br⁻, XPS analysis was conducted on all\nground samples (Fig. R2-2 to 2-6). The relative atomic percentages of Br obtained from\nXPS showed a trend similar to that derived from EDS analysis, reinforcing the critical\nrole of the cation source in the bromine substitution process. A notable discrepancy was\nobserved for the S-KBr sample, where the Br percentage differed significantly between\nEDS (bulk-sensitive) and XPS (surface-sensitive) measurements. This suggests a lower\nefficiency of bromine substitution in S-KBr, with Br⁻ predominantly located near the\nsample surface. Conversely, for the S-CsBr, S-MABr, S-FABr, and S-GuaBr samples,\nthe consistent Br percentages from both techniques indicate a more substantial\nincorporation of Br⁻ into the bulk phase.\nFig. R2-2 The XPS spectra of Cl 2p (a) and Br 3d (b) for the S-KBr sample.\nFig. R2-3 The XPS spectra of Cl 2p (a) and Br 3d (b) for the S-CsBr sample.\nFig. R2-4 The XPS spectra of Cl 2p (a) and Br 3d (b) for the S-GuaBr sample.\nFig. R2-5 The XPS spectra of Cl 2p (a) and Br 3d (b) for the S-MABr sample.\nFig. R2-6 The XPS spectra of Cl 2p (a) and Br 3d (b) for the S-FABr sample.\nTable. R2-1 The percentage of Br in the sample relative to the total halogen content\nBr/Cl+Br S-KBr S-CsBr S-MABr S-FABr S-GuaBr\nEDS 12.72% 69.77% 93.48% 85.51% 90.73%\nXPS 44.27% 71.96% 84.71% 74.20 % 83.75%\nIn summary, the combined EDS and XPS data conclusively demonstrate the effective\nand cation-dependent incorporation of Br⁻ into the material's structure via the grinding\nprocess, with organic cations facilitating more profound and homogeneous substitution.\nThe corresponding figures and discussions are supplemented into the manuscript and\nSI.\nComment 2-2. The authors state that the ground samples form new crystalline phases,\nyet the manuscript does not provide any data on their long-term or environmental\nstability. Since these materials are proposed for optoelectronic applications, the authors\nshould clarify whether the CPL intensity, PLQY, and SHG efficiency remain stable\nunder ambient conditions (air, humidity, light exposure) or degrade over time.\nResponse 2-2：We sincerely thank the reviewer for the valuable comment regarding\nsample stability. As suggested, we have re-prepared the samples and systematically\nevaluated their stability after being stored under ambient temperature (25°C), ambient\nlight, and low-humidity conditions (20% RH) for 14 days. The results demonstrate that\nthe retention rates of the key optoelectronic properties, namely circularly polarized\nluminescence (CPL) intensity, second-harmonic generation (SHG) intensity, and\nphotoluminescence quantum yield (PLQY), all exceeded 95% (Fig. R2-7 to 2-9 and\nTable R2-2). This conclusively indicates that the samples possess excellent short-term\nstability under room temperature and low-humidity conditions, providing crucial\nexperimental support for their practical storage and potential application. We fully\nacknowledge the importance of long-term stability assessments, which represents a key\nfocus for our future research.\nFig. R2-7 The stability of CPL properties of a R/S-InSb, b R/S-KBr, c R/S-CsBr, d\nR/S-GuaBr, e R/S-MABr and f R/S-FABr.\nFig. R2-8 The stability of SHG intensity of a S-InSb, b S-KBr, c S-CsBr, d S-GuaBr,\ne S-MABr and f S-FABr.\nFig. R2-9 The PLQY of a S-InSb, b S-KBr, c S-CsBr, d S-GuaBr, e S-MABr and f S-\nFABr.\nFig. R2-10 The stability of PLQY of a S-InSb, b S-KBr, c S-CsBr, d S-GuaBr, e S-\nMABr and f S-FABr after 14 days.\nTable. R2-2 The PLQY of the samples before and after grinding\nS-InSb S-KBr S-CsBr S-MABr S-GuaBr S-FABr\nComment 2-3. In Figure 1c, the presented XRD pattern seems to correspond to InSb,\nbut the discussion in line 76 mainly focuses on the phosphorescent properties of R/S-\nIn. It would be helpful if the authors could clearly indicate in the figure caption or text\nwhich sample the XRD data represent, to avoid possible confusion.\nResponse 2-3: We sincerely thank the reviewer for this careful observation and the\nvaluable suggestion to improve the clarity of our figure presentation. We apologize for\nany confusion caused by the original labeling and context. We have already emphasized\nthe correspondence between the description and Figure 1c, and have also highlighted\nthe annotations for the XRD samples in Figure 1c to distinguish them.\nComment 2-4. In the main text (lines 79-80), Figure S2 is described as showing the\nCD spectrum of R/S-In, whereas the actual Figure S2 in the supplementary information\nappears to present the CD spectrum of InSb. The figure and the text should be aligned.\nResponse 2-4: We sincerely thank the reviewer for this meticulous observation and for\nbringing this discrepancy to our attention. We sincerely apologize for the error and any\nconfusion it caused in the original submission. The reviewer is absolutely correct. To\naddress this issue thoroughly and ensure full alignment between the main text and the\nSupporting Information, we have added the correct Figure S2. This new figure is now\ncorrectly labeled as Figure S2. And the caption for the new Figure S2 reads: \"Fig. S2.\nThe CD spectrum of R/S-In.\" All the subsequent figures in SI sections has been checked\nand corrected.\nComment 2-5: Due to the missing Figure S2 (In CD spectrum), all subsequent\nsupplementary figures seem to have been shifted by one position (e.g., what is labeled\nas S3 should actually be S2). The figure numbering in the supplementary section should\nbe carefully checked and corrected.\nResponse 2-5: Thanks to the valuable suggestions from the reviewers. The submitted\nversion indeed has the mistake. We have corrected the main text and SI to make sure\nall the figures and tables are matched in this version. These suggestions have\nsignificantly improved the accuracy and clarity of our paper.\nComment 2-6. In line 98, the text refers to “Fig. 1b,” but it should correspond to “Fig.\n1c.” The figure citation should be corrected.\nResponse 2-6: Thanks to the careful observation of the reviewers, we have carefully\nrevised the citations in Figure 1b and Figure 1c. At the same time, we have carefully\nchecked and verified the correspondence between the citations in the full text and the\nfigures.\nComment 2-7. In Figure S12, the sample is labeled as “MA,” although it represents\nMABr. The notation should be corrected to “MABr” for consistency with the figure\ncaption and the main text.\nResponse 2-7: Thank the reviewers for their careful pointing out of this issue. This will\nsignificantly enhance the accuracy and rigor of our manuscript. In the supporting\ninformation, we have changed the label of the sample from “S-MA” to “S-MABr”.\nComment 2-8. The authors suggest that stronger hydrogen bonding with small cations\n(e.g., Gua+) enhances chiral transfer. However, the manuscript does not provide\nexperimental evidence verifying the stronger hydrogen bonding in GuaBr. It is more\nlikely that Gua+ introduces additional NH donors rather than intrinsically stronger H-\nbonds. Comparison with pure GuaBr and pure MABr samples would clarify whether\nthe observed effects result from hydrogen-bond network reconstruction or simply from\nthe presence of organic bromide species.\nResponse 2-8: We thank the reviewer for highlighting the need for evidence of\nhydrogen bond evolution. we have performed additional Raman spectroscopy tests on\npure GuaBr and MABr salts and systematically compared them with the spectra of the\nsamples before and after grinding. The results provide further clarification on the roles\nof these organic cations.\nIn the GuaBr grinding system, the characteristic sharp peak of pure GuaBr observed\nat 3317 cm⁻¹ undergoes a distinct shift to a higher wavenumber region (3328 cm⁻¹) upon\ngrinding, accompanied by noticeable peak broadening (Fig. R2-11). This observation\nindicates that the Gua⁺ cation plays a dual role in the post-grinding sample: it acts not\nonly as a hydrogen bond donor but also contributes to the reconstruction and\nenhancement of the hydrogen bonding network. We will refine our description\nregarding the role of GuaBr in strengthening hydrogen bonding to reflect this finding\nmore accurately.\nIn the MABr grinding system, the characteristic peak of pure MABr in the C-H\nstretching vibration region (2961 cm⁻¹) shifts to a lower wavenumber (2950 cm⁻¹) in\nthe ground S-MABr sample (Fig. R2-14). Furthermore, a distinctly broadened peak\nemerges in the 3200-3600 cm⁻¹ region. These spectral changes demonstrate that MABr\nalso plays a significant role in the reconstruction of the hydrogen bonding network.\nThe corresponding figures and discussions are supplemented into the manuscript and\nSI.\nFig. R2-11 The Raman spectra of S-InSb, GuaBr and S- GuaBr.\nFig. R2-12 The Raman spectra of S-InSb, MABr and S- MABr.\nComment 2-9. In lines 182–184, Cl– is introduced without prior explanation. The\nauthors should clarify earlier that the pristine material (InSb) is composed of In–Cl\noctahedra and specify the origin of Cl– before discussing Br⁻ substitution.\nResponse 2-9: We sincerely thank the reviewer for this critical observation regarding\nthe need for clarity on the chemical composition of the pristine material and the origin\nof the Cl⁻ ions. We agree that establishing this foundational information early in the\nmanuscript is essential for the reader to fully comprehend the subsequent discussion on\nBr⁻ substitution. We have carefully addressed this point in the revised manuscript.\n“……, indicating that the chiral ligands have successfully transferred chirality between\nthe In-Cl octahedral structures.” (Lines 82-83)\n“In the crystal structure of S-InSb, the chiral structure is composed of In-Cl octahedra\nand chiral ligands.” (Line 234-235)\nThese modifications ensure that the origin of Cl⁻ and the chloride-based nature of the\npristine material are unambiguously communicated to the reader before the concept of\nBr⁻ substitution is introduced. This sequential presentation of information, first defining\nthe initial state then describing its modification, significantly improves the logical flow\nand scientific rigor of the manuscript. We believe these changes have fully addressed\nthe reviewer's valuable concern and have enhanced the clarity of our work. Thank you\nagain for this helpful suggestion.\nComment 2-10. The authors state that in S-MABr, MA+ does not enter the lattice and\nthat Cl– is replaced by Br– after grinding, forming N–H···Br hydrogen bonds. If the\nnewly formed hydrogen bonds are indeed responsible for the opposite chiral\narrangement, it should be clarified whether such Br– substitution also occurs in the other\nbromide salts (KBr, CsBr, GuaBr, FABr), or if Cl– remains in those cases. This point is\ncrucial, as the enhanced SHG response is also explained by Br– substitution.\nResponse 2-10: We thank the reviewer for raising this critical point regarding the\nuniversality of Br⁻ substitution and its role in hydrogen bond formation across different\nbromide salts. To address this, we have performed additional Raman spectroscopy\nmeasurements on the ground samples (S-KBr, S-CsBr, S-MABr, S-GuaBr, S-FABr) in\nthe 3200–3600 cm⁻¹ region (Fig. R2-13), which directly probes N–H/O–H stretching\nvibrations and provides insights into hydrogen bonding interactions. The results are\nsummarized in the figure below and offer clarifying evidence.\nFor inorganic Bromide Salts (S-KBr, S-CsBr): Both samples show negligible peaks\nin this region, similar to the pristine S-InSb. This indicates that grinding with KBr or\nCsBr does not lead to significant formation of new N–H∙∙∙Br hydrogen bonds. We\nattribute this to the absence of hydrogen bond donors (e.g., N–H or O–H groups) in\ninorganic cations (K⁺, Cs⁺). While Br⁻ substitution may still occur at the halogen sites\n(as supported by XPS/EDS data), the lack of organic cations prevents the reconstruction\nof a hydrogen bond network, thus explaining the absence of Raman peaks in this region.\nFor organic Bromide Salts (S-MABr, S-GuaBr, S-FABr): In contrast, all organic salts\nexhibit distinct spectral features: S-MABr displays a broad characteristic peak centered\naround 3300 cm⁻¹, consistent with the formation of a dynamic N–H∙∙∙Br hydrogen bond\nnetwork after Br⁻ substitution. S-GuaBr and S-FABr also show peaks in this region, but\nwith distinctly different peak shapes and positions compared to S-MABr. For instance,\nS-GuaBr exhibits a sharper peak at ~3328 cm⁻¹, while S-FABr shows a broadened\nenvelope with variations in intensity distribution. This indicates that while Br⁻\nsubstitution occurs in all cases (as confirmed by XPS/EDS), the specific hydrogen\nbonding network reconstructed depends strongly on the organic cation (e.g., size,\nfunctional groups, and hydrogen-bonding capability of MA⁺, Gua⁺, and FA⁺)\nImplications for Br⁻ Substitution and SHG Enhancement: The occurrence of bromide\nion substitution in the sample was confirmed by XPS, EDS, and Raman data. However,\ndue to the differences in cations, the degree of bromide ion substitution and the strength\nof hydrogen bonding are not exactly the same. The enhanced second harmonic\ngeneration response is driven by the structural changes caused by the combined effects\nof bromide ion substitution and hydrogen bonding generated by cations. We have\nrevised the manuscript to reflect these subtle differences. Thank you for promoting this\nmore in-depth analysis.\nS-InSb S-KBr S-CsBr\nS-MABr S-GuaBr S-FABr\ny\nt\ni\ns\nn\ne\nt\nn\nI\n3200 3300 3400 3500 3600\nRaman Shift (cm-1)\nFig. R2-13 The Raman spectra of S-InSb, S-KBr, S-CsBr, S-GuaBr, S-MABr and S-\nFABr.\nComment 2-11. In line 270, the manuscript reports maximum g values of\nlum\napproximately 1.37 × 10–2 and -1.98 × 10–2, but it is unclear from which sample these\nvalues were obtained. The authors should specify the measurement source and include\nthe corresponding CPL (g ) spectra in the Supporting Information for clarity.\nlum\nResponse 2-11: We sincerely thank the reviewer for this meticulous observation and\nfor identifying the lack of clarity regarding the source of the maximum g values\nlum\nreported in our original manuscript (line 270). We apologize for this oversight in data\nreferencing. We have thoroughly addressed this issue in the revised manuscript to\nensure complete transparency and accuracy.\nThe maximum g values of approximately +1.37 × 10⁻² and -1.98 × 10⁻² originate\nlum\nfrom the CP-LED devices fabricated using the R-GuaBr and S-GuaBr samples,\nrespectively. We have explicitly stated this source in the main text (now around line\n334) to avoid any ambiguity. The original phrasing has been revised to: \"Notably, the\nCP-LED devices fabricated with the ground R-GuaBr and S-GuaBr samples exhibited\nthe maximum |g | values of approximately +1.37 × 10⁻² and -1.98 × 10⁻²,\nlum\nrespectively.\" As suggested, we have now included the complete CPL spectra (and the\ncorresponding g spectra calculated from them) for the R/S-GuaBr-based CP-LED\nlum\ndevices in the Supporting Information as Figure S30. This provides a clear visual\nrepresentation of the data from which these maximum values were extracted.\nFig. R2-14 The g value of R/S-GuaBr-based CP-LED devices.\nlum\nComment 2-12. As the samples are powder forms of single crystal, it is difficult to\nmeasure CPL and CD of these samples. Please explain how the authors made samples\nand took measurements?\nResponse 2-12: We sincerely thank the reviewer for raising this important\nmethodological point regarding the measurement of Circularly Polarized Luminescence\n(CPL) and Circular Dichroism (CD) for powder samples. We fully agree that obtaining\nreliable chiroptical data from powdered crystalline materials can be challenging due to\nissues like light scattering. To address this fundamental concern and ensure the highest\ndata quality, we employed a well-established thin-film preparation protocol for these\nspecific measurements. The detailed procedure is as follows.\nSample Preparation for CPL/CD Measurements: The powder was dissolved\nanhydrous N, N-Dimethylformamide (DMF) under mild stirring to form a clear,\nhomogeneous solution. The solution was then spin-coated onto meticulously cleaned\nquartz substrates. The spin-coating parameters were rigorously controlled: a speed of\n2000 revolutions per minute (rpm) for a duration of 30 seconds. Immediately after spin-\ncoating, the films were transferred to a hotplate and annealed at 100 °C for 10 minutes.\nThe corresponding discussions are supplemented into the experimental section of the\nmanuscript.\nComment 2-13. In CP-LED applications, are all UV excitation light absorbed by singe\ncrystals? If not, there should be some leakage lights which are not absorbed by the\nsingle crystals.\nResponse 2-13: We sincerely thank the reviewer for raising this critical point regarding\nthe completeness of UV light absorption in our CP-LED device configuration. The\nreviewer is absolutely correct. We acknowledge that in our experimental setup, not all\nUV excitation light is absorbed by the sample layer; a portion of the UV light is indeed\nscattered or transmitted, leading to some leakage. In our CP-LED devices, the sample\nwere mixed with polydimethylsiloxane (PDMS) and then coated onto a commercial\nUV-LED chip (365 nm). While the sample layer is designed to absorb the UV light, its\nfinite thickness and the scattering nature of the powder mean that complete (100%)\nabsorption is challenging to achieve in practice. Therefore, some degree of UV light\nleakage is an inherent characteristic of this type of device architecture, as correctly\npointed out by the reviewer.\nReviewer #3 (Remarks to the Author):\nThis manuscript presents a highly innovative and significant study on the post-synthetic\nregulation of chiral indium-based metal halides using a simple grinding strategy. The\n\"Midas touch\" approach demonstrates remarkable versatility, enabling multifaceted\nmodulation of key optical properties—including CPL amplification, inversion, NIR\nemission, and a dramatic enhancement of SHG. The work showcases compelling\napplications in CP-LEDs, logic gates, and anti-counterfeiting. Generally speaking, this\nwork is meticulously executed, and the findings are of significant interest. It may worth\nthe attention of the readership of Nature Communications if the following points are\nappropriately addressed.\nComment 3-1. Is the effect unique to bromide salts? Control experiments with chloride\nor iodide salts (e.g., KCl) would be highly informative to delineate whether anion\nexchange (Cl⁻ to Br⁻) is the primary driver or if cations and mechanical force play more\ncomplex roles. This is crucial, as halogen substitution has been shown to significantly\nalter optical properties in chiral metal halides.\nResponse 3-1：We sincerely thank the reviewer for this insightful suggestion. To\ndirectly address whether the observed effects are unique to bromide salts and to\ndelineate the roles of anion exchange versus cations, we have performed comprehensive\ncontrol experiments by grinding S-InSb with a series of chloride and iodide salts\npossessing the same cationic counterparts (K⁺, Cs⁺, MA⁺, FA⁺, Gua⁺). The resulting PL\nspectra are summarized in the Fig. R3-1 below, and they provide crucial insights.\nFig. R3-1 a PL photos of the S-InSb and the samples after grinding treatment wih\nchloride and b iodate salts under 365 nm ultraviolet light irradiation. c-h The PL\nspectra of S-InSb, S-KBr, S-KCl, S -CsBr, S-CsCl, S -MABr, S-MACl, S-GuaBr, S-\nGuaCl, S-FABr and S-FACl.\nOur control experiments reveal that the effect is not unique to bromide salts, but\nbromide salts consistently induce the most pronounced changes. The results highlight\na complex interplay between the halide anion (X⁻) and the cation (A⁺) during the\nmechanochemical process:\nChloride and Bromide Salts Induce Cation-Dependent Spectral Shifts: More\nimportantly, grinding with chloride salts (Fig. R3-1a) also induces significant shifts in\nthe PL spectrum compared to pristine S-InSb, confirming that anion exchange (Cl⁻ for\nCl⁻/Br⁻) is not the sole driver. The direction and magnitude of the shift (blue or red) are\nstrongly influenced by the cation: For salts with the same cation, Br⁻ substitution\nconsistently induces a larger spectral shift (blue or red) than Cl⁻ substitution (S-FABr\nvs. S-FACl). This demonstrates that Br⁻ is more effective in modulating the electronic\nstructure (e.g., band gap or STE energy level), likely due to its appropriate ionic radius\nand electronegativity.\nIodide Salts Cause PL Quenching: As shown in Fig. R3-1b, grinding S-InSb with\nany of the iodide salts (e.g., CsI, MAI, FAI, GuaI) results in complete or near-complete\nquenching of the PL signal. This suggests that the large ionic radius of I⁻ disrupts the\noriginal crystal structure of S-InSb during grinding, preventing the formation of a stable,\nluminescent phase. This observation underscores that successful modification requires\ncompatible halide ionic radii.\nThe cation itself dictates the trend of the shift. For example, S-KCl and S-KBr both\ncause a blue shift, while S-FACl and S-FABr both cause a red shift. Notably, for cations\nof intermediate size (MA⁺, Gua⁺), chloride salts lead to a blue shift, whereas their\nbromide counterparts result in a red shift. This crossover effect powerfully demonstrates\nthat the cation is not a passive spectator but plays an active and synergistic role in the\nstructural outcome.\nSynergistic Role of Cations Linked to Ionic Radius: The observed trends in PL shifts\ncan be rationalized by considering the ionic radius series: K⁺ < Cs⁺ < MA⁺ < FA⁺ <\nGua⁺. We propose that the size of the cation, in conjunction with the halide, influences\nthe packing and strain within the newly formed organic-inorganic hybrid structure\nduring grinding, thereby cooperatively tuning the optical properties.\nIn conclusion, these control experiments decisively show that while halogen\nexchange is a primary driver (with Br⁻ being most effective), the cation plays a critical\nand complex synergistic role. The optical properties of the ground product are\ndetermined by the specific A⁺/X⁻ pair. This deeper understanding, gained entirely from\nthe reviewer's suggestion, significantly strengthens our mechanistic interpretation. We\nhave incorporated these findings and the corresponding discussion into the revised\nmanuscript\nComment 3-2. The achievement of NIR CPL without rare-earth metals or I⁻ ions is\nsignificant. It is better to expand the discussion on how the grinding with FABr\nspecifically modifies the STE states or band structure to enable such a large Stokes shift\nand NIR emission, potentially referencing relevant studies on STE emission in metal\nhalides.\nResponse 3-2: We sincerely thank the reviewer for this insightful comment regarding\nthe underlying mechanism enabling near-infrared (NIR) circularly polarized\nluminescence (CPL) in the S-FABr sample. We agree that a deeper discussion on how\ngrinding with FABr modifies the self-trapped exciton (STE) states is crucial. Based on\nthe reviewer's suggestion, we have performed and analyzed temperature-dependent\nphotoluminescence (PL) experiments for S-FABr. The results, summarized in the figure\nbelow, provide compelling evidence for the STE mechanism and allow us to elaborate\non the specific role of the FABr grinding process. The corresponding figures and\ndiscussions are supplemented into the manuscript and SI.\nFig. R3-2 a Temperature-dependent fluorescence spectrum of S-FABr. b\nPL/temperature correlation map of S-FABr upon excitation at 360 nm, respectively, as\nthe temperature varied from 260 to 340 K. c Temperature-dependent full width at half\nmaximum (FWHM) of S-FABr. d Temperature-dependent PL intensity of S-FABr.\nAs shown in Figs. R3-2a and R3-2b, the PL intensity of S-FABr decreases\nsignificantly with increasing temperature (thermal quenching). Concurrently, the full\nwidth at half maximum (FWHM) of the emission band broadens considerably with\ntemperature (Fig. R3-2c). This combination of strong thermal quenching and\nprogressive linewidth broadening is a hallmark of emission originating from STEs,\nwhere the excitons are strongly coupled to the lattice vibrations.\nTo quantitatively assess the electron-phonon coupling strength, we fitted the\ntemperature-dependent FWHM data. The obtained Huang-Rhys factor (S) is 30.25,\nwhich is significantly larger than 5. This large S value unambiguously indicates very\nstrong electron-phonon coupling in the ground S-FABr material. Such strong coupling\nis a prerequisite for the formation of STEs and the associated large Stokes shift. The\nactivation energy (Ea) for thermal quenching, derived from the Arrhenius plot in Fig.\nR3-2d, is 138.50 meV. This value represents the stability of the self-trapped state. It\nfalls within a range that is conducive to STE formation at room temperature—\nsufficiently high to stabilize the STEs, leading to the observed NIR emission.\nℏ𝜔\n𝐹𝑊𝐻𝑀(𝑇) = 2.36√𝑆ℏ𝜔 √𝑐𝑜𝑡ℎ\n𝑝ℎ𝑜𝑛𝑜𝑛\n(1)\n𝑝ℎ𝑜𝑛𝑜𝑛 2𝑘 𝑇\n𝐵\n𝐼\n0\n𝐼(𝑇) = (2)\n𝐸\n1+𝐴𝑒𝑥𝑝(− 𝑎 )\n𝑘 𝑇\n𝐵\nComment 3-3. In Figure 3b, d, e, the CPL spectra of the ground samples (e.g., R/S-\nKBr, R/S-GuaBr, R/S-MABr) are not perfectly symmetrical. This asymmetry may\nindicate a change in the emission mechanism or the presence of multiple emitting\nspecies with different chiral environments. Please provide the corresponding total\nfluorescence (DC) spectra and give a plausible explanation for this phenomenon.\nResponse 3-3: We sincerely thank the reviewer for this keen observation regarding the\nasymmetry in the CPL spectra of the samples (R/S-KBr, R/S-GuaBr, R/S-MABr) in\nFigures 3b, d, and e. We appreciate the opportunity to clarify this point. To investigate\nthis possibility, we provide the corresponding total fluorescence spectra (DC spectra)\nfor the R- and S-enantiomers of each ground sample, as requested. The DC spectra for\nthe R- and S-enantiomers of each pair (KBr, GuaBr, MABr) exhibit a strong mirror-\nimage relationship with respect to the intensity axis. This indicates that the ground\nsamples are enantiopure and that the fundamental photoluminescence mechanisms for\nthe two chiral forms are essentially identical and symmetric. As the reviewer astutely\nnoted from the raw data, we do observe very minor peak position differences between\nsome R/S pairs in the DC spectra upon precise fitting, specifically:\nR-KBr (601 nm) vs. S-KBr (596 nm) - Δλ = 5 nm\nR-GuaBr (631 nm) vs. S-GuaBr (634 nm) - Δλ = 3 nm\nR-MABr (635 nm) vs. S-MABr (639 nm) - Δλ = 4 nm\nTo delve deeper into this issue, we systematically re-measured the CPL spectra of\nall the ground samples. Each sample was independently measured five times and the\naverage spectra were calculated (Fig. R3-4 to 3-8). The average CPL spectra of all\nenantiomer pairs exhibited excellent mirror symmetry. The symmetrical averaged CPL\nspectra strongly proved that each ground sample had a single, dominant chiral\nenvironment, and the luminescence originated from a single chiral species rather than\nmultiple different chiral environments with luminescent species. To further confirm the\nhomogeneity of the samples and the reliability of the chiral optical data, we conducted\nangle-dependent CPL measurements (Fig. R3-9). When rotating the samples, no\nsignificant changes in the spectral line shape were detected. Based on these findings,\nwe replaced the original single-scan CPL spectra in Figure 3 of the manuscript with the\naverage spectra. Furthermore, the g values corresponding to the spectrum have also\nlum\nbeen updated in the supporting information. These new figures correctly demonstrate\nthe inherent symmetry of the samples. We thank the reviewers for raising this issue,\nwhich prompted our data presentation to be more rigorous and accurate.\nFig. R3-3 The CPL spectra (upper) and the Corresponding DC spectra (below) of a\nR/S-KBr, b R/S-GuaBr and c R/S-MABr.\nFig. R3-4 The CPL spectra of a R/S-InSb, b R/S-KBr, c R/S-CsBr, d R/S-GuaBr, e\nR/S-MABr and f R/S-FABr with 5 cycles of measurements.\n800\nm ) R/S-FABr\nn\n(700\nh R/S-GuaBr\ng t R/S-CsBr R/S-MABr\nn R/S-InSb\ne\nl R/S-KBr\ne600\nv\na\nW\nS-InSb R-KBr S-CsBrR-GuaBr S-MABrR-FABr\nFig. R3-5 The error bar of the CPL spectra of a R/S-InSb, b R/S-KBr, c R/S-CsBr, d\nR/S-GuaBr, e R/S-MABr and f R/S-FABr with 5 cycles of measurements.\nFig. R3-6 The averaged CPL spectra of a R/S-InSb, b R/S-KBr, c R/S-CsBr, d R/S-\nGuaBr, e R/S-MABr and f R/S-FABr with 5 cycles of measurements.\nFig. R3-7 The DC spectra of R/S-InSb, R/S-KBr, R/S-CsBr, R/S-GuaBr, R/S-MABr\nand R/S-FABr.\nFig. R3-8 The g of R/S-InSb, R/S-KBr, R/S-CsBr, R/S-GuaBr, R/S-MABr and\nlum\nR/S-FABr.\nFig. R3-9 The CPL spectra of a R/S-InSb, b R/S-KBr, c R/S-CsBr, d R/S-GuaBr, e\nR/S-MABr and f R/S-FABr from multiple angles.\nComment 3-4. Several figures in SI are cited incorrectly. Please review them to ensure\naccurate citations throughout the manuscript.\nResponse 3-4: We sincerely thank the reviewer for this meticulous observation\nregarding the citation inaccuracies of figures in the Supporting Information (SI). We\ndeeply apologize for these oversights, which occurred during the complex process of\nintegrating a large amount of characterization data and multiple rounds of manuscript\nrevision. The manuscript and the Supporting Information has been comprehensively\nrevised to ensure that all citations to figures, tables, and other elements are now accurate.\nComment 3-5. Some recently published related papers may be of reference value, e.g.,\n10.1021/acs.accounts.3c00599, 10.1002/anie.202308194.\nResponse 3-5: We are grateful to the reviewers for recommending these two important\npapers (Acc. Chem. Res. 2023, DOI: 10.1021/acs.accounts.3c00599; Angew. Chem. Int.\nEd. 2023, DOI: 10.1002/anie.202308194). After careful reading, we believe they are of\ngreat reference value and have included them in our references.\nComment 3-6. The manuscript contains a few typographical errors, grammatical\nmistakes, and occasionally awkward phrasing that detract from the scientific narrative.\nTo meet the high publication standard, a comprehensive line-by-line revision is\nrecommended of the entire manuscript.\nResponse 3-6: We sincerely thank the reviewer for this critical comment regarding the\nlanguage quality of our manuscript. We fully agree that clear and precise scientific\nexpression is essential for communicating our findings effectively. In direct response to\nthis feedback, we have conducted a comprehensive, line-by-line revision of the entire\nmanuscript and marked it in blue font, with the primary goal of enhancing readability,\ngrammatical accuracy, and the overall flow of the scientific narrative."}, {"round": 2, "reviewer_comments": {"reviewer_1": "After careful evaluation of revised manuscript, I believe that the manuscript can be suitable for publication in journal “Nature Communications” in presented form. All necessary additions and clarifications are made in the revised manuscript.", "reviewer_2": "The authors addressed well the reviewer's comments. One minor comment is the authors need to define \"R/S-In\" when it is firstly used in the manuscript. If the authors address this minor comments, the reviewer recommends publication of this manuscript.", "reviewer_3": "The authors have adequately revised their manuscript according to my previous comments and suggestions. The quality of the manuscript has been improved after the revision. The revised manuscript is recommended for publication in its present form."}, "author_response": ""}]

Decision letter