DOI: 10.5061/dryad.n8pk0p316
title: Room-temperature quantum coherence of entangled multiexcitons in a metal-organic framework

description: Singlet fission (SF) can generate an exchange-coupled quintet triplet pair
 state 5TT, which could lead to the realization of quantum computing and
 quantum sensing using entangled multiple qubits even at room temperature.
 However, the observation of the quantum coherence of 5TT has been limited
 to cryogenic temperatures, and the fundamental question is what kind of
 material design will enable its room-temperature quantum coherence. Here
 we show that the quantum coherence of SF-derived 5TT in a
 chromophore-integrated metal-organic framework (MOF) can be over hundred
 nanoseconds at room temperature. The subtle motion of the chromophores in
 ordered domains within the MOF leads to the enough fluctuation of the
 exchange interaction necessary for 5TT generation, but at the same time
 does not cause severe 5TT decoherence. Furthermore, the phase and
 amplitude of quantum beating can be controlled by molecular motion,
 opening the way to room-temperature molecular quantum computing based on
 multiple quantum gate control.
description: # Title of Dataset Room-temperature quantum coherence of entangled
 multiexcitons in a metal-organic framework [Access this dataset on
 Dryad](10.5061/dryad.n8pk0p316) Links to publications that cite or use the
 data: Yamauchi, K. Tanaka, M. Fuki, S. Fujiwara, N. Kimizuka, T. Ryu, M.
 Saigo, K. Onda, R. Kusumoto, N. Ueno, H. Sato, Y. Kobori, K. Miyata, N.
 Yanai, Room-temperature quantum coherence of entangled multiexcitons in a
 metal-organic framework, Sci. Adv. 2024, 10, eadi3147.
 Experimental
 details are written in the paper. File list: Fig2B.xlsx Fig2C.xlsx
 Fig3.xlsx Fig. 4A.csv Fig4A_100ns_10us_sim.csv Fig4C_nsTA150Kexp.csv
 Fig4C_nsTA150Ksim.csv Fig6C.csv Fig6C_sim.csv Fig6D.csv Fig6D_sim.csv
 Fig6E_rev.csv Data_Fig6F.csv FigS1.xlsx FigS3.xlsx FigS4.xlsx FigS5.xlsx
 Data_figS6A.csv Data_figS6B.xlsx Data_FigS7AB.csv FigS8.xlsx FigS8_sim.csv
 Data_FigS9AB.csv Data_FigS10A.csv Data_FigS10B.csv Data_FigS10C.csv
 FigS11_A_C.csv FigS12B.csv FigS13_MOF_Pc_RT_3Ddata_4us.csv
 FigS15_Nutation_profile.csv FigS15_FT_spect.csv FigS16B.csv FigS16C.csv
 FigS16C_fit.csv FigS16D.csv FigS16D_fit.csv FigS18_THz_MOF_data.csv
 Relationship between files: Written in each data (If it exists)
 Abbreviations: MOF: Metal-Organic Framework PXRD: Powder X-Ray Diffraction
 UV-vis: Ultraviolet-visible TA: Transient Absorption Spectroscopy TAS:
 Transient Absorption Spectroscopy EAS: Evolution Assisted Spectra abs:
 absorption CW-TREPR: Continuous-Wave Electron Paramagnetic Resonance EPR:
 Electron Paramagnetic Resonance TGA: Thermogravimetric Analysis STP:
 Standard Temperature and Pressure FFT: Fast Fourier Transform THz:
 Terahertz Pn-MOF and PDBA are names of the samples used in this research.
 Pn-MOF is a MOF consisited by PDBA (molecules) and zirconium cluster.
 Measurements were conducted in neat conditions of each sample, dispersed
 in paraffin, or in DMF (dimethylformamide) solution. ## Description of the
 data and file structure --- DATA-SPECIFIC INFORMATION FOR: Fig2B.xlsx
 Variable List: 2theta (degree): the diffraction angle of each samples in
 PXRD Intensity (a.u.): the signal intensity of each samples in PXRD ---
 DATA-SPECIFIC INFORMATION FOR: Fig2C.xlsx Variable List: Wavelength (nm)
 :the measurement wavelength in UV-visible absorption measurements
 Intensity (a.u.) : the signal intensity of each samples in UV-visible
 absorption measurements --- DATA-SPECIFIC INFORMATION FOR: Fig3.xlsx For
 Fig3A Variable List: Wavelength (nm): the wavelength of each data at each
 time time (ps): the time that took the transient absorption spectra
 Delta_abs (a.u.): the absorption changes at each time in ns-TAS
 measurements For Fig3B Variable List: time (ps): the time that took the
 data Delta_abs (a.u.): the time profile of absoption changes of
 experimental and fitted data at 485 nm and 530 nm in ns-TAS measurements
 For Fig3C Variable List: Wavelength (nm): the measurement wavelength at
 each time in ns-TAS measurements EAS (a.u.): the evolution assisted
 spectra of the first component (S1) and the second component (TT) in
 ns-TAS measurements For Fig.3D Variable List: Time (ns): the time that
 took the data Delta_abs_530 (a.u.): the time profile of absoption changes
 at 530 nm at 300 K and 150 K --- DATA-SPECIFIC INFORMATION FOR: Fig.
 4A.csv and Fig4A_100ns_10us_sim.csv Fig4A_100ns_10us_sim.csv is simulated
 spectra of Fig4A.csv Variable List: Magnetic field (mT): the magnetic
 field of each data time (µs): the time that take the spectra, 0.1-10 us
 were shown Intensity (a.u.): the intensity of CW-TREPR signals ---
 DATA-SPECIFIC INFORMATION FOR: Fig4C_nsTA150Kexp.csv,
 Fig4C_nsTA150Ksim.csv, Fig4C_nsTA300Kexp.csv and Fig4C_nsTA300Ksim.csv
 Fig4C_nsTA150Ksim.csv and Fig4C_nsTA300Ksim.csv are the simulated data of
 each corresponding experimental data (same as Fig.3D). the third and
 fourth columns mean the changes derived from 5TT and (T+T) state. Variable
 List: Time (ns): the time that took the data Delta_abs_530 (a.u.): the
 time profile of absoption changes at 530 nm at 300 K and 150 K ---
 DATA-SPECIFIC INFORMATION FOR: Fig6C.csv and Fig6C_sim.csv Fig6C_sim.csv
 is simulated spectra of Fig6C.csv. Variable List: Magnetic field (mT): the
 magnetic field of each data Intensity (a.u.): the intensity at each
 magnetic field --- DATA-SPECIFIC INFORMATION FOR: Fig6D.csv and
 Fig6D_sim.csv Fig6D_sim.csv is simulation of Fig6D.csv. The last two raws
 of the simulation data mean the nutation profile from ?0,±1and ?±2,±1
 tranditions, respectively. Variable List: Nutation pulse duration (ns):
 the duration of nutation pulse sequence of each data Intensity (a.u.): the
 intensity of pulsed EPR signal (correspond to y-magnetization) with each
 duration --- DATA-SPECIFIC INFORMATION FOR: Fig6E_rev.csv The second and
 third columns means nutation profile considering with the dihedral angle
 change between 130 degree to 122 degree and 130 degree to 150 degree,
 respectively. Variable List: Nutation pulse duration (ns): the duration of
 nutation pulse sequence of each data Intensity (a.u.): the intensity of
 pulsed EPR signal (correspond to y-magnetization) with each duration ---
 DATA-SPECIFIC INFORMATION FOR: Data_Fig6F.csv Variable List: Time (ns):
 the time that took each data Intensity (a.u.): the time profile of
 CW-TREPR intensity (the second column) and the echo intensity (the fourth
 column; simulated and sixth column; experimental) --- DATA-SPECIFIC
 INFORMATION FOR: FigS1.xlsx Variable List: Wavenumber (cm-1): the
 wavenumber that took each data Transmittance (a.u.): the transmittance of
 each samples in FT-IR measurements --- DATA-SPECIFIC INFORMATION FOR:
 FigS3.xlsx Variable List: Temperature (Celsius degree): the temperature
 that took each data Weight loss (%): the weight loss of the sample in TGA
 --- DATA-SPECIFIC INFORMATION FOR: FigS4.xlsx Adsorption and desorption
 process were separated. Variable List: Relative pressure (p/p0, relative
 pressure to saturation vapor pressure): the relative pressure that took
 each data N2 uptake (cm3 (STP) g-1): the N2 uptake of the MOF ---
 DATA-SPECIFIC INFORMATION FOR: FigS5.xlsx Data taken at each temperature
 were separated in different tabs. Variable List: Wavelength (nm): the
 wavelength that took the data Time (ns): the time that took the data
 Delta_mOD (a.u.): the absorption changes at each wavelength in ns-TAS
 measurements --- DATA-SPECIFIC INFORMATION FOR: Data_figS6A.csv and
 Data_figS6B.xlsx Variable List: Magnetic field (mT): the magnetic field of
 each data Orientation change (degree) : The change of relative dihedral
 angle between two pentacenes Intensity (a.u.): the simulated EPR intensity
 at each magnetic field with each orientation change --- DATA-SPECIFIC
 INFORMATION FOR: Data_FigS7AB.csv The EPR spectra considering with only
 130 and 150 degrees pair (second column), weighted average of 130 and
 150+-20 degrees pair (third column), and weighted average of 130+-20 and
 150 degrees pair (fourth column). Variable List: Magnetic field (mT): the
 magnetic field of each data Intensity (a.u.): the simulated EPR intensity
 at each magnetic field with each orientation --- DATA-SPECIFIC INFORMATION
 FOR: FigS8.xlsx and FigS8_sim.csv FigS8_sim.csv is simulated spectra of
 FigS8.xlsx. Variable List: Magnetic field (mT): the magnetic field of each
 data Intensity (a.u.): the EPR intensity at each magnetic field ---
 DATA-SPECIFIC INFORMATION FOR: Data_FigS9AB.csv The EPR spectra
 considering with 125 and 150, 140, 130, 120, 100, 90, 110 degrees pair and
 its weighted average. Variable List: Magnetic field (mT): the magnetic
 field of each data Orientation change (degree) : the change of relative
 dihedral angle between two pentacenes Intensity (a.u.): the simulated EPR
 intensity at each magnetic field with each orientation change ---
 DATA-SPECIFIC INFORMATION FOR: Data_FigS10A.csv, Data_FigS10B.csv, and
 Data_FigS10C.csv The time profile of EPR spectra considering with weighted
 average of 130 and 150 degrees pair (FigS10A), weighted average of 125 and
 110 degrees pair (FigS10B), and their summed spectra (FigS10C) Variable
 List: Magnetic field (mT): the magnetic field of each data Time (µs): the
 time that took the data Intensity (a.u.): the simulated EPR intensity at
 each magnetic field with each orientation change --- DATA-SPECIFIC
 INFORMATION FOR: FigS11_A_C.csv The second column is data of FigS11A and
 the third column is data of FigS11C, respectively. Variable List: Magnetic
 field (mT): the magnetic field of each data Intensity (a.u.): the
 simulated EPR intensity at each magnetic field with each orientation
 change --- DATA-SPECIFIC INFORMATION FOR: FigS12B.csv The second column is
 simulated data of Fig S4C at room temperature considering with only TT
 diffusion. The third and fourth columns mean the changes derived from 5TT
 and (T+T) state. Variable List: Time (ns): the time that took the data
 Delta_abs_530 (a.u.): the time profile of absoption changes at 530 nm at
 300 K and 150 K --- DATA-SPECIFIC INFORMATION FOR:
 FigS13_MOF_Pc_RT_3Ddata_4us.csv Each columns are correspond with the data
 of each magnetic fields. Each rows are correspond with the data of each
 times. Variable List: Time (ns): the time that took the data Magnetic
 field (mT): the magnetic field of each data Intensity (a.u.): the EPR
 intensity at each magnetic field and time --- DATA-SPECIFIC INFORMATION
 FOR: FigS15_Nutation_profile.csv and FigS15_FT_spect.csv
 FigS15_Nutation_profile.csv is data of FigS15A and FigS15_FT_spect.csv is
 data of FigS15B. For FigS15_Nutation_profile.csv, the second and fourth
 columns are the raw data and processed data. The third column are apllied
 window function for the data processing. Variable List: Time (ns): the
 time that took the data Frequency (MHz): the nutation frequency of each
 data Intensity (a.u.): the EPR and FFT intensity at each magnetic field
 and time --- DATA-SPECIFIC INFORMATION FOR: FigS16B.csv Variable List:
 Time (ns): the time that took the data Intensity (a.u.): the EPR intensity
 at each magnetic field and time --- DATA-SPECIFIC INFORMATION FOR:
 FigS16C.csv, FigS16C_fit.csv, FigS16D.csv, and FigS16D_fit.csv
 FigS16C_fit.csv and FigS16D_fit.csv are mono-exponential fits of each
 corresponding data. Variable List: tau_echo (ns): the pulse duration time
 of each data Intensity (a.u.): the EPR intensity at each duration time ---
 DATA-SPECIFIC INFORMATION FOR: FigS18_THz_MOF_data.csv The second column
 and third column are correspond to FigS18A and Fig S18B, respectively.
 Variable List: Wavenumber (cm-1): the wavenumber of each data Intensity
 (a.u.): the intensity of each data in teraheltz measurements