# Rational Construction of Layered Two-Dimensional Conjugated Metal–Organic Frameworks with Room-Temperature Quantum Coherence

Yang Lu, Yubin Fu, Ziqi Hu, Shiyi Feng, Morteza Torabi, Lei Gao, Shuai Fu, Zhiyong Wang, Chuanhui Huang, Xing Huang, et al.

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Yang Lu, Yubin Fu, Ziqi Hu, Shiyi Feng, Morteza Torabi, et al.. Rational Construction of Layered Two-Dimensional Conjugated Metal–Organic Frameworks with Room-Temperature Quantum Coherence. Journal of the American Chemical Society, 2025, 147 (10), pp.8778-8784. 10.1021/jacs.4c18681. hal-04987734

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# Rational Construction of Layered Two-Dimensional Conjugated Metal–Organic Frameworks with Room-Temperature Quantum Coherence

Yang Lu,✉ Yubin Fu,✉ Ziqi Hu,* Shiyi Feng, Morteza Torabi, Lei Gao, Shuai Fu, Zhiyong Wang, Chuanhui Huang, Xing Huang, Mingchao Wang, Noel Israel, Evgenia Dmitrieva, Hai I. Wang, Mischa Bonn, Paolo Samorì, Renhao Dong,* Eugenio Coronado,* and Xinliang Feng*

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Cite This: J. Am. Chem. Soc. 2025, 147, 8778–8784

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Supporting Information

**ABSTRACT:** Two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have emerged as an intriguing class of quantum materials due to their high crystallinity, persistent spin centers, and tunable structures and topologies. However, it remains unclear how to achieve long spin relaxation time at room temperature in 2D c-MOFs via a bottom-up design strategy. Herein, we design a hexahydroxytrithiatruxene ligand (HHTH) to minimize the influence of nuclear spin on electron spin relaxation while weakening $d-\pi$ conjugation to construct a “spin docking” for preserving spin centers, which enables the resulting 2D c-MOFs, $Ni_3HHTH_2$, to exhibit quantum coherence and Rabi oscillations at room temperature. Spin dynamics studies not only reveal an unusual temperature-dependent Rabi frequency in $Ni_3HHTH_2$ but also indicate that the coordination mode determines the spin–lattice relaxation behavior via spin–phonon coupling. These investigations provide a general guideline for the development of high-performance quantum qubits based on 2D spin arrays.

<figure><img src="image_9.png" /><figcaption>“Spin docking”
in 2D c-MOFs</figcaption></figure>

✓ Low H atoms occupation

✓ Nuclear spin-free coordination

<figure><img src="image_10.png" /><figcaption>Room Temperature</figcaption></figure>

<caption>Quantum Coherence and Rabi Oscillation</caption>

## INTRODUCTION

Over the past decade, two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have emerged as a new type of $d-\pi$ conjugated van der Waals layered materials, attracting increasing attention due to their unique combination of porosity and electrical conductivity.¹⁻⁹ Significantly, the redox coordination polymerization reaction between $\pi$-conjugated ligands featuring adjacent substituent atoms (N, O, and S) and metal ions lead to the creation of persistent radicals on these ligands, endowing 2D c-MOFs with a distinct identity as “spin-concentrated assemblies.”¹⁰⁻¹² Compared to organic/inorganic molecular spin materials, spin centers in 2D c-MOFs not only exhibit excellent air stability, weak spin–orbit coupling, and hyperfine interactions, but also, more importantly, allow for scalable tuning of spin dynamics.¹³⁻¹⁵ These preliminary explorations position 2D c-MOFs as promising candidates for quantum materials.¹⁰,¹⁶ However, the strong interlayer coupling, combined with intralayer $d-\pi$ conjugation, accelerates spin relaxation across the entire framework.¹⁷ The consequent low spin concentration (the number of unpaired electron spins per unit of the material) and rapid spin relaxation severely limit the potential of 2D c-MOFs as robust spin qubit arrays.

The dynamics of molecular spins are predominantly governed by their surrounding chemical environment, characterized by

two key processes: (i) energy transfer between the spin and its environment (e.g., the 'lattice'), quantified by the spin–lattice relaxation time ($T_1$); and (ii) spin decoherence, described by the quantum coherence time ($T_2$).¹⁴,¹⁵,¹⁸ In principle, modulating the $d-\pi$ conjugated structures of 2D c-MOFs, which constitute the local connection sphere of the spin, could significantly influence the spin distribution, thereby controlling the spin relaxation process.¹⁰ On the other hand, the spin-dephasing process is susceptible to losses induced by nuclei, such as hydrogen or nitrogen atoms in the conjugated framework, through hyperfine interactions between electrons and nuclear spins.¹⁶,¹⁹⁻²⁵ Up to now, it is still highly challenging to develop molecular design strategies toward long spin–lattice and spin-decoherence times at room temperature in 2D c-MOFs.¹³,¹⁷

Herein, we report a novel 2D c-MOF based on a $\pi$-conjugated ligand, benzo[1,2–b:3,4–b’:5,6–b’]tris[1]benzothiophene–2,3,7,8,12,13-hexol (HHTH), which possesses a similar $\pi$-

Received: December 30, 2024

Revised: February 13, 2025

Accepted: February 18, 2025

Published: February 27, 2025

<figure><img src="image_11.png" /></figure>
<figure><img src="image_12.png" /><figcaption>**Figure 1.** Rational design concept of Ni₃HHTH₂ and Ni₃HATI₂ 2D c-MOFs (top). Comparison of key static and dynamic spin properties between Ni₃HHTH₂ and Ni₃HATI₂ 2D c-MOFs (bottom table).</figcaption></figure>

<figure><img src="image_13.png" /><figcaption>**Figure 2.** Structural characterization of Ni₃HHTH₂ and Ni₃HATI₂. (a–b) Pawley refinement of PXRD data with experimental (gray), simulated (red), and difference (blue) patterns for Ni₃HHTH₂ and Ni₃HATI₂. HRTEM images of Ni₃HHTH₂ with fast Fourier transform analysis of the corresponding areas: (c) imaged along the *c* direction and (d) imaged normal to the *c* direction. (e) Schematic stacking mode of Ni₃HHTH₂ and Ni₃HATI₂.</figcaption></figure>

conjugated structure to the previously reported 2,3,7,8,12,13-hexaiminotiindole (HATI) ligand (Figure 1).¹³ Nuclear spin-free Ni²⁺ is utilized to link the HHTH or HATI ligands, resulting in the formation of the corresponding 2D c-MOFs, Ni₃HHTH₂ and Ni₃HATI₂, respectively, which exhibit identical topology and interlayer stacking modes. Compared to Ni₃HATI₂, Ni₃HHTH₂ has 60% fewer hydrogen atoms; and nuclear spin-free oxygen and sulfur atoms replace the nitrogen atoms with nuclear spin in Ni₃HATI₂. Theoretical calculations indicate that the [NiO₄] secondary building units (SBUs) of Ni₃HHTH₂ can serve as a “spin dock”, effectively localizing the spin center and shielding it from rapid relaxation. Pulse electron paramagnetic resonance (EPR) spectroscopy elucidates the spin dynamics of Ni₃HHTH₂, with T₁ and T₂ values of 5.6 µs and 164 ns at 300 K,

which are comparable with those of classical MOF-based qubits.¹³ An unusual temperature-dependent Rabi frequency is further revealed, which is attributed to the coupling of electron spins to phonons.

## ■ RESULTS AND DISCUSSION

The conjugated ligand, HHTH with C₃ symmetry was synthesized through a modified cyclotrimerization of 5,6-dimethoxybenzo[b]thiophen-3(2H)-one and further demethylation reactions (refer to the SI for synthesis details). Ni₃HHTH₂ was then constructed under solvothermal conditions by reacting HHTH with Ni(acac)₂ in a 3:1 (v/v) mixture of H₂O and dimethylacetamide (DMAc) in a glass vial at 85 °C for 12 h. The synthesis conditions for Ni₃HATI₂ were
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<figure><img src="image_17.png" /><figcaption>**Figure 3.** (a) Electrical conductivities of Ni₃HHTH₂ and Ni₃HATI₂ in the temperature range of 200–320 K. (b) THz photoconductivity dynamics following 3.1 eV photoexcitation (pump fluence: 760 µBCJ/cm²). Bulk spin density distributions for (c) Ni₃HHTH₂ and (d) Ni₃HATI₂, and the yellow and cyan colors denote α and β spin densities, whose iso-value is 0.005 e/Bohr³.</figcaption></figure>

optimized based on the previous report²⁶ (see the SI Section S2). X-ray photoelectron spectroscopy (XPS) analysis of the Ni(2p) regions reveals the presence of Ni(II) in both 2D c-MOFs (Figures S1–S2). Fourier transform infrared (FT-IR) spectroscopy reveals the near disappearance of O–H and N–H stretching vibration bands belonging to the ligand in both Ni₃HHTH₂ and Ni₃HATI₂ (Figure S3), indicating the deprotonation and subsequent formation of Ni–O and Ni–NH coordination bonds, respectively. Thermogravimetric analysis (TGA) reveals that both 2D c-MOFs start desolvation over 100 °C and exhibit pronounced weight losses above 200 °C due to decomposition (Figure S4). Scanning electron microscopy (SEM, Figure S5) showed rod-like nanocrystals.

Powder X-ray diffraction (PXRD) analysis of Ni₃HHTH₂ revealed a crystalline phase, evidenced by prominent peaks at 2θ = 3.74, 6.58, 7.57, 10.00, 16.84, and 27.40° (Figure 2a). The PXRD of Ni₃HATI₂ (Figure 2b) has a similar pattern to Ni₃HHTH₂. The structural elucidation for both samples was achieved through simulation and Pawley refinement of the PXRD experimental data with unit cell parameters listed in Table S1. Comparison of the PXRD pattern and density functional theory (DFT) simulations unveils a long-range growth in the ab plane, accompanied by a serrated layered arrangement characterized by an interlayer shift of 0.1*a and 0.1*b (Figure 2e). The broad peaks centered around 2θ = 27.40° correspond to the (002) plane, revealing an interlayer spacing of ~3.25 Å in both MOFs. The local structures of the samples were further confirmed by high-resolution transmission electron microscopy (HRTEM). The fast Fourier transform (FFT) analysis of HRTEM images of Ni₃HHTH₂ and Ni₃HATI₂ presents a honeycomb lattice with a lattice distance of 25.4 Å (Figures 2c–d and S6), which is consistent with the

PXRD and calculated results. N₂ adsorption isotherms at 77 K indicate Brunauer–Emmett–Teller (BET) surface areas of 960 and 1080 m² g⁻¹ for Ni₃HHTH₂ and Ni₃HATI₂, respectively (Figure S7). Both samples possess the average pore size of 2.1 nm obtained by fitting the isotherm, which agrees with the predicted pore structure with diameters of ~2.1 nm. The achieved results further prove that these samples are isostructural 2D c-MOFs.

Optical absorption reveals that Ni₃HHTH₂ exhibits a larger optical bandgap (0.40 eV) than that of Ni₃HATI₂ (0.25 eV) (Figure S8). This observation suggests a significant difference in the spin bath of organic radicals generated through coordination of conjugated ligands with Ni ions. The parallel four-probe measurements under ambient conditions showed that the electrical conductivities of Ni₃HHTH₂ and Ni₃HATI₂ powder pellets at 298 K are 1.6 ± 0.2 × 10⁻² S cm⁻¹ and 1.1 ± 0.1 S cm⁻¹, respectively (Figure 3a). Both samples exhibit thermally activated charge transport according to the variable-temperature (VT) conductivity measurements from 200 to 320 K. The activation energy for charge transport in Ni₃HHTH₂ is 238 meV, significantly higher than the 45 meV observed in Ni₃HATI₂. This substantial disparity further suggests notable differences in charge transport behavior between two isostructural 2D c-MOFs.

To investigate their microscopic transport properties, we employed time-resolved terahertz spectroscopy (TRTS, see SI for details). Ni₃(HHTH)₂ and Ni₃(HATI)₂ both exhibit a rapid sub-ps rise in photoconductivity due to the quasi-instantaneous injection of free carriers (Figure 3b). This is followed by a ps-level decay, attributed to exciton formation, electron–hole recombination and/or defect trapping.²⁷,²⁸ The substantial difference in the photoconductivity amplitude provides
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<figure><img src="image_20.png" /><figcaption>**Figure 4.** (a) Continuous-wave (CW) EPR spectra of Ni₃HHTH₂ and Ni₃HATI₂ measured at 300 K. (b) CW-EPR spectra of Ni₃HHTH₂ measured at 10–300 K. (c) Temperature dependence of T₁ and T₂ for Ni₃HHTH₂ and the fits see text. (d) Normalized echo intensity in nutation experiments using different attenuation powers of the applied microwave at 300 K on Ni₃HHTH₂. (e) Nutation experiments on Ni₃HHTH₂ at different temperatures using the fixed microwave attenuation power of 12 dB. (f) Temperature dependence of Rabi frequencies determined by nutation experiments at different attenuation powers. The solid lines are guides for the eye.</figcaption></figure>

preliminary evidence of their distinct charge transport proper-
ties. Further analysis on the frequency-resolved complex
photoconductivity Δσ(ω) by the phenomenological Drude–
Smith (DS) model reveals a substantial difference in the charge
scattering time (τ) (~1–10 fs for Ni₃HHTH₂ and 150 ± 10 fs
for Ni₃HATI₂), which partially explains the photoconductivity
discrepancy. The calculated band structures reveal that the band
dispersion near the Fermi level along the π-stacking direction in
Ni₃HATI₂ is significantly larger than in Ni₃HHTH₂, indicating
that Ni₃HATI₂ has considerably stronger interlayer electronic
coupling and therefore more efficient carrier transport than
Ni₃HHTH₂ (Figures S9–S10). The spin distributions obtained
from DFT calculations also differ notably between Ni₃HHTH₂
and Ni₃HATI₂ (Figures 3c–d and S11), with the spin in
Ni₃HATI₂ being significantly more delocalized across the entire
d–π conjugated framework (including the H atoms) compared
to Ni₃HHTH₂. These results suggest that the extended spin
carriers in Ni₃HATI₂ interact with the high gyromagnetic ratio
H nuclei along transport pathways, simultaneously increasing
the likelihood of spin interactions across layers, which may
enhance the spin relaxation process. Combined with spin
distribution analysis, it is evident that the [NiO₄] linker in
Ni₃HHTH₂ acts as a trap in charge transport, resulting in lower
transport efficiency. On the other hand, it may also function as a
spin docking site, which prevents the spin centers from
decoherence. These characteristics can be beneficial for
achieving high spin concentration and ultralong spin lifetimes
in spin qubit arrays.

X-band continuous-wave (CW) EPR spectroscopy was first
utilized to probe the spin centers in these 2D c-MOFs. The CW

EPR spectrum of Ni₃HHTH₂ at room temperature (300 K) displays a single resonance peak at *g* = 2.0063 with a peak-to-peak line width of 5 G. In contrast, a peak at *g* = 2.0052 is identified for Ni₃HATI₂ with a much larger line width up to 17 G (Figure 4a). According to the Elliott mechanism, the scattering of high-conduction carriers by phonons in Ni₃HATI₂ results in a shortened spin–lattice relaxation time, thereby broadening the EPR signals. This strongly suggests that the spin centers in Ni₃HHTH₂ are more localized.²⁹ This observation also implies that Ni₃HHTH₂ exhibits a longer spin lifetime. Quantitative EPR analysis reveals that Ni₃HHTH₂ possesses a spin concentration of 1.3 × 10²¹ mol⁻¹, nearly an order of magnitude higher than that of Ni₃HATI₂. VT-EPR spectra of the spin-concentrated Ni₃HHTH₂ show that the spin signal becomes more intense as temperature decreases (Figure 4b). Doubly integrating the EPR spectra, the temperature dependence of spin susceptibility χₜₜₜ in a χₜₜₜ T–T plot showcases a clear slope at the temperature region of 50–300 K, revealing significant Pauli contributions from free conducting electrons (Figure S12).

Next, we employed the pulsed EPR technique to characterize
the spin dynamics of Ni₃HHTH₂ on dry powders. Intriguingly,
spin echo signals can be detected at room temperature. Using
inversion recovery and Hahn echo decay pulse sequences, T₁
and T₂ were determined to be 5.6 µs and 164 ns at 300 K,
respectively, demonstrating long-lived radical centers in a spin-
concentrated 2D c-MOF. Such an excellent spin decoherence
property is comparable with those of classical MOF-based
qubits,¹³ while the vast majority of MOF-based qubits show
fragile quantum coherence predominantly at low temper-
ature.¹⁵,¹⁷,³⁰ In comparison, the spin echo signal for Ni₃HATI₂
is too weak to be recorded even at 5 K due to the highly delocalized radicals over [NiNH₄] and hyperfine coupling with abundant hydrogen atoms in the framework. Upon cooling, the value of T₁ of Ni₃HHTH₂ first increases and then becomes nearly temperature-independent below 20 K, reaching up to 158 µs at 6 K (Figure 4c). On the other hand, T₂ remains almost constant and thus is not limited by T₁ in the whole temperature range of 6–300 K since T₁ is sufficiently longer. A similar observation has been reported for molecular graphene nanostructures, which suggests that decoherence likely stems from electron–electron scattering along the π-stacks.³¹ The above-mentioned results point out that the introduction of spin docking sites in 2D c-MOFs, although significantly reducing electrical conductivity from 1.1 S cm⁻¹ down to 0.016 S cm⁻¹, markedly enhances spin concentration from 1.9 × 10²⁰ mol⁻¹ to 1.3 × 10²¹ mol⁻¹ and achieves room-temperature quantum coherence. This highlights an important design principle for developing 2D c-MOF-based spin qubits.

The temperature dependence of T₁ for Ni₃HHTH₂ is fitted by considering cross-relaxation, Raman-like, and local-mode processes using the following expression:

$$T_1^{-1} = A_{\text{Cross}} + A_{\text{Raman}} T^n + A_{\text{Loc}} \frac{\exp(h\nu/T)}{(\exp(h\nu/T) - 1)^2}$$

where the first cross-relaxation term is temperature-independent arising from spin–spin interaction,³² the second term denotes a power law of the two-phonon Raman mechanism,³³ and the third term describes the circumstance when a local vibrational mode with a frequency of ν is responsible for spin relaxation via spin–phonon coupling.³⁴ Extracted from this analysis, an excellent simulation is obtained with A<sub>Cross</sub> = 6.28 × 10³ s⁻¹, A<sub>Raman</sub> = 2.62 s⁻¹K⁻¹ and n = 1.87 for the Raman-like mechanism, which is attributed to the spin–phonon bottleneck effect,³⁵ as well as A<sub>Loc</sub> = 8.81 × 10⁵ s⁻¹ and ν = 604 cm⁻¹ consistent with the excitation energy (~606 cm⁻¹) of local stretching mode of the Ni–O bonds observed by IR spectroscopy (Figure S13). Note that a combination of cross-relaxation and Raman-like mechanism alone is not able to produce a satisfactory fit in the high-temperature region of 150–300 K (Figure 4c), demonstrating the crucial role of the local vibrational mode in governing spin relaxation of Ni₃HHTH₂ at high temperatures.

Nutation experiments of Ni₃HHTH₂, showing Rabi oscillation decays (Figure 4d), confirm that arbitrary superposition of spin states can be generated at room temperature with appropriate microwave pulses, establishing Ni₃HHTH₂ as an excellent S = 1/2 spin qubit candidate for quantum gate operations (Figures S14–S18). This phenomenon is corroborated by the quantitative analysis of spin concentration in Ni₃HHTH₂, which reveals that only about 1% of the conjugated ligands contain radicals. This leads to negligible interactions between spin centers, resulting in properties characteristic of nearly isolated free radicals. The Fourier transform of nutation experiments confirms the Rabi oscillations with Rabi frequency Ω<sub>Rabi</sub> proportional to the magnetic field B₁ of the applied microwave pulse, satisfying the Rabi relationship ħΩ<sub>Rabi</sub> = gu<sub>B</sub>SB₁, where ħ is the reduced Planck constant and µ<sub>B</sub> is the Bohr magneton. Surprisingly, temperature-dependent Rabi frequency is observed in Ni₃HHTH₂ above 150 K, despite the temperature-independent Rabi relationship (Figure 4e–f). This behavior is likely attributed to phonon-induced renormalization of Rabi frequency, a phenomenon previously reported for

optically driven semiconducting quantum dots.³⁶,³⁷ Such an unprecedented behavior in electron spin qubits suggests strong spin–phonon coupling in this 2D c-MOF, likely driven by the local vibrational mode identified from the temperature dependence of T₁ at similarly high temperatures.

## CONCLUSIONS

In summary, we report a novel 2D c-MOF, Ni₃HHTH₂ based on a π-conjugated ligand hexahydroxytrithiatruxene ligand by incorporating nuclear spin-free S and O atoms to construct “spin docking” SBU in a 2D d-π conjugated system. Ni₃HHTH₂ exhibits quantum coherence and Rabi oscillations at room temperature. Spin dynamics studies indicate that Ni–O bonds stretching vibration, a local vibrational mode, is crucial for spin–lattice relaxation at high temperatures above 150 K via spin–phonon coupling. This local mode is likely also responsible for the first observation of phonon-induced temperature-dependent Rabi frequency in electron spin qubits. Our simple yet effective bottom-up design strategy provides an approach to developing high-performance spin qubits based on 2D spin arrays. Precisely controlling the spin concentration in 2D c-MOFs and exploring the concentration-dependent spin dynamics remain the focus of our future efforts.

## ASSOCIATED CONTENT

### Supporting Information

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c18681.

Experimental methods, characterization data, NMR spectra, TEM images, SEM images, XPS spectra, DFT calculations, conductivity measurements, and EPR measurements (PDF)

## AUTHOR INFORMATION

### Corresponding Authors

Ziqi Hu – Instituto de Ciencia Molecular (ICMol), Universitat de València, 46980 Paterna, Spain; Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, Anhui Laboratory of Advanced Photon Science and Technology, University of Science and Technology of China, 230026 Hefei, China; ● orcid.org/0000-0003-1830-1584; Email: huziqi@ustc.edu.cn

Renhao Dong – Department of Chemistry, The University of Hong Kong, Hong Kong 999077, China; Materials Innovation Institute for Life Sciences and Energy (MILES), HKU-SIRI, Shenzhen 518048, China; ● orcid.org/0000-0002-4125-9284; Email: rhdong@hku.hk

Eugenio Coronado – Instituto de Ciencia Molecular (ICMol), Universitat de València, 46980 Paterna, Spain; ● orcid.org/0000-0002-1848-8791; Email: eugenio.coronado@uv.es

Xinliang Feng – Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany; Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany; ● orcid.org/0000-0003-3885-2703; Email: xinliang.feng@tu-dresden.de

### Authors

Yang Lu – Université de Strasbourg, CNRS, ISIS, UMR 7006, 67000 Strasbourg, France; Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany; Center for Advancing Electronics Dresden & Faculty of
Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany; MOE Key Laboratory of Low-grade Energy Utilization Technologies and Systems, School of Energy & Power Engineering, Chongqing University, 400044 Chongqing, China; orcid.org/0000-0001-9416-2198

Yubin Fu - Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany; orcid.org/0000-0002-2613-394X

Shiyi Feng - Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany

Morteza Torabi - Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany

Lei Gao - Max Planck Institute for Polymer Research, 55128 Mainz, Germany

Shuai Fu - Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany; Max Planck Institute for Polymer Research, 55128 Mainz, Germany

Zhiyong Wang - Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany; Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany; orcid.org/0000-0002-0909-9495

Chuanhui Huang - Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany

Xing Huang - Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany

Mingchao Wang - Max Planck Institute of Microstructure Physics, 06120 Halle (Saale), Germany; Center for Advancing Electronics Dresden & Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01067 Dresden, Germany; Present Address: School of Advanced Materials, Peking University, Shenzhen Graduate School, 518055 Shenzhen, China; orcid.org/0000-0001-9979-3503

Noel Israel - Leibniz Institute for Solid State and Materials Research, 01069 Dresden, Germany

Evgenia Dmitrieva - Leibniz Institute for Solid State and Materials Research, 01069 Dresden, Germany; orcid.org/0000-0001-7490-617X

Hai I. Wang - Max Planck Institute for Polymer Research, 55128 Mainz, Germany; Nanophotonics, Debye Institute for Nanomaterials Science, Utrecht University, 3584 CC Utrecht, The Netherlands; orcid.org/0000-0003-0940-3984

Mischa Bonn - Max Planck Institute for Polymer Research, 55128 Mainz, Germany; orcid.org/0000-0001-6851-8453

Paolo Samorì - Université de Strasbourg, CNRS, ISIS, UMR 7006, 67000 Strasbourg, France; orcid.org/0000-0001-6256-8281

Complete contact information is available at:
https://pubs.acs.org/10.1021/jacs.4c18681

Author Contributions

Y.L. and Y.F. contributed equally to this work. All authors have given approval to the final version of the manuscript.

Notes

The authors declare no competing financial interest.

ACKNOWLEDGMENTS

Y.L. and P.S. thanks Marie Skłodowska-Curie Fellowship (T2DMOF, No. 101103585). This work is financially supported by DFG projects (CRC-1415, No. 417590517; RTG 2861, No. 491865171), ERC starting grant (FC2DMOF, No. 852909), ERC Consolidator Grant (T2DCP, No. 819698) as well as the German Science Council and Center of Advancing Electronics Dresden (cfaed). The authors acknowledge cfaed and Dresden Center for Nanoanalysis (DCN) at TUD. R.D. thanks the National Natural Science Foundation of China (22272092 & 22472085), the Taishan Scholars Program of Shandong Province (tsqn201909047), and Natural Science Foundation of Shandong Province (ZR2023JQ005). We gratefully acknowledge the GWK support for funding this project by providing computing time through the Centre for Information Services and HPC (ZIH) at TU Dresden.

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