Quan-Song Li's research while affiliated with Beijing Institute of Technology and other places

Publications (61)

Article
Aggregation-induced emission (AIE) materials with photocyclization (PC) reactions exhibit rich photophysical and photochemical activities. Understanding the mechanism behind is essential to the design of effective AIE materials. Herein, we employ a polarizable continuum model (PCM) and the hybrid quantum mechanics and molecular mechanics (QM/MM) ap...
Article
Molecular engineering has been demonstrated to be a predominant strategy for augmenting the long-term stability and passivating adverse defects for perovskite solar cells (PSCs). Here, using density functional theory calculations combined with ab initio molecular dynamics (AIMD) simulations, the passivation effects of bidentate passivation molecule...
Article
The first reversible photoisomerization between a borepin and a borirane was reported in the photo‐induced reactions of B(npy)Ar 2 (npy=2‐(naphthalen‐1‐yl) pyridine, Ar=phenyl or electron rich aryl). (S. Wang, et al. Angew. Chem. Int. Ed. 2019 , 58 , 66836687). In this work, the detailed mechanisms of the unprecedented reversible photoisomerization...
Article
Sulfinyl radicals (R-SO˙) play important roles in lots of reactions, while the isomer oxathiyl radicals (R-OS˙) and the isomerization between them are rarely observed due to the poor stability of R-OS˙. In this work, the complete active space self-consistent field (CASSCF) and its multi-state second order perturbation (MS-CASPT2) methods were emplo...
Article
Contemporary perovskite solar cells (PSCs) have drawn substantial interest due to their high photovoltaic efficiency. However, the instability of perovskite in a humid environment restricts the service time extension and limits the large‐scale application of PSCs. Herein, a series of passivation molecules (PMs), 2‐MEP, 2‐MDEP, 2‐MTEP, and 2‐MQEP, f...
Article
Full-text available
The acceptors play vital roles in absorbing sunlight and consequently producing charge in organic solar cells (OSCs). Boron-based non-fullerene acceptors have received particular attention due to their tunable electronic structure...
Article
In the field of synthetic organic materials, there is still an urgent demand for new smart materials that show great potential in diverse applications. We herein describe a design strategy for the synthesis of luminescent organoboranes (M1,M2andM3) that feature a central eight-membered octacyclic scaffold with an electron donor (Ar3N) and acceptor...
Article
Chemical passivation implemented by Lewis base has been demonstrated as an effective method to overcome the water vulnerability of perovskite solar cells (PSCs) along with better performance. Comprehensive understanding of the surface passivation effects is crucial to future improve the PSCs efficiency and stability. Herein, we utilized first-princ...
Article
Full-text available
The acceptor in organic solar cells (OSCs) is of paramount importance for achieving a high photovoltaic performance. Based on the well-known non-fullerene acceptor Y6, we designed a set of asymmetric A-D1A'D2-A type new acceptors Y6-C, Y6-N, Y6-O, Y6-Se, and Y6-Si by substituting the two S atoms of one thieno[3,2-b]thiophene unit with C, N, O, Se,...
Article
Organic azides are an efficient source of nitrenes, which serve as vigorous intermediates in many useful organic reactions. In this work, the complete active space self-consistent field (CASSCF) and its second-order perturbation (CASPT2) methods were employed to study the photochemistry of 2-furoylazide 1 and 3-furoylazide 5, including the Curtius...
Article
Full-text available
As the key component of organic solar cells (OSCs), the acceptor plays key roles in determining the power conversion efficiency (PCE). Based on the famous non-fullerene acceptor ITIC, a series of acceptors (A1-A5) were designed by introducing fused-ring units (phenanthrene, pyrene, benzopyrazine, dibenzo[a,c]phenazine, and phenanthro[4,5-abc]phenaz...
Article
The electron transporting material (ETM) in inverted perovskite solar cells (PSCs) play important roles in reducing hysteresis and realizing simple processing procedures, while the improvement of power conversion efficiency is limited by the low electron mobility and weak perovskite/ETM interface interaction. In this work, three new ETMs (HAT-1, HA...
Article
N, C‐chelate organoboron compounds are widely employed as photo‐responsive and optoelectronic materials due to their efficient photochromic reactivity. It was found in experiments that two diphenyl substituted organoboron compounds, B(ppy)Ph 2 (ppy=2‐phenylpyridyl) and B(iba)Ph 2 (iba=N‐isopropyl‐benzylidene‐amine), display distinct photochemical r...
Article
As the first discovered organoboron compound with photochromic property, B(ppy)Mes 2 (ppy=2‐phenylpyridine, Mes=mesityl) displays rich photochemistry that constitutes a solid foundation for wide applications in optoelectronic fields. In this work, we investigated the B(ppy)Mes 2 to borirane isomerization mechanisms in the three lowest electronic st...
Article
The reaction of 1,1,2,2-tetrakis(4-(pyridin-4-yl)phenyl)ethene (tppe) with [Fe(NCBH3)2] produced a two-dimensional coordination polymer [Fe(NCBH3)2(tppe)] n (1), which was pillared in an ABAB manner through interlayer multiple [C-Hδ+···Hδ--B] dihydrogen bonds (DHBs) to form a stable porous three-dimensional (3D) supramolecular structure that showed...
Article
In inverted perovskite solar cells (PSCs), electron transfer materials (ETMs) have a significant effect on the efficiency and stability, because they can reduce the energy barrier between perovskite film and electrode materials and suppress the potential interfacial charge recombination. Herein we designed a series of ETMs (o-PDTP, m-PDTP, and p-PD...
Article
Electronic structure calculations and nonadiabatic dynamics simulations were carried out on excited state decay mechanism of a typical AIE‐active molecule THBDBA, which was experimentally found almost non‐emissive in solution but highly luminescent as an aggregate. At MS‐CASPT2//CASSCF level, the decay path from S1 leads to a conical intersection (...
Article
The complete active space self-consistent field (CASSCF) and its second-order perturbation (CASPT2) methods combining with time-dependent density functional theory (TD-DFT) have been employed to investigate the isomerization reaction mechanisms of an asymmetric N,C-chelate organoboron compound B(ppy)MesPh in ground (S0) state and the first singlet...
Article
Acceptor-π-donor-π-acceptor (A-π-D-π-A) type small molecule acceptors have made significant progress in organic solar cells (OSCs). To achieve high performance acceptors, three novel acceptors (s4-s6) are designed and investigated based on small molecule acceptors (s1-s3) via introduction of different end-capped groups. The quantum chemistry and Ma...
Article
Development of a simple and stable photocatalyst for overall water splitting is a promising avenue for solar energy conversion. Here, carbon nitride nanosheets (CN) panel decorated with in situ formed (111) facets-oriented Au nanoparticles (AuNPs) have been prepared by vapor-deposition polymerization (VDP) followed with easy immersion technique. Be...
Article
Suitable electron transport material (ETM) plays key roles in efficient perovskite solar cells (PSCs), because it is beneficial to exciton dissociation and charge transport at the interface thus increasing the short circuit current density. Based on the experimentally reported efficient electron transport molecule 10,14-bis(5-(2-ethylhexyl)thiophen...
Article
Borverbindungen. In der Zuschrift auf S. 9782 berichten Q.‐S. Li, S. Wang et al. über die Photoisomerisierung von chiralen Organoborverbindungen zu N,B,X‐Heterocyclen durch Bor‐Insertion in die C‐X‐Bindung (Bild: Nikolas Mancuso).
Article
Boron Compounds. Q.‐S. Li, S. Wang et al. describe the conversion of chiral organoboranes into N,B,X‐heterocycles in an excited‐state process that involves boron insertion into the C−X bond in their Communication on page 9634 ff. (Graphic: Nikolas Mancuso.)
Article
Acceptor-π-donor-π-acceptor (A-π-D-π-A) type of small molecules is very promising nonfullerene acceptors to overcome the drawbacks of the fullerene derivatives such as the weak absorption ability and electronic adjustability. However, few attempts have been done to develop -bridge unit to construct highly efficient acceptors in OSCs. Herein, takin...
Article
Chiral organoboron compounds with a chelate backbone and mesityl/heterocycle substituents on boron (thienyl, furyl and derivatives) undergo a quantitative phototransformation yielding rare, chiral N,B,X‐embedded heterocycles (b) (e.g. base‐stabilized 1,2‐thiaborinines and 1,2‐oxaborinines). Boriranes (a) were observed as intermediates in some of th...
Article
Chiral organoboron compounds with a chelate backbone and mesityl/heterocycle substituents on boron (thienyl, furyl and derivatives) undergo a quantitative phototransformation yielding rare, chiral N,B,X‐embedded heterocycles (b) (e.g. base‐stabilized 1,2‐thiaborinines and 1,2‐oxaborinines). Boriranes (a) were observed as intermediates in some of th...
Article
Full-text available
Arylchlorodiazirines (ACDA) are thermal and photochemical precursors of carbenes that form these molecules both via nitrogen elimination. We have studied this reaction with multireference quantum chemical methods (CASSCF and CASPT2) for a series of ACDA derivatives with different substitution at the aromatic ring. The calculations explain the diffe...
Article
As the simplest and the most abundant dicarboxylic acids in the atmosphere, oxalic acid (OA) not only plays a key role in aerosol nucleation, but also acts as a prototypical compound for the investigation of intra- and intermolecular hydrogen bonding interactions. In this work, a systematic theoretical study on the hydrated OA dimers were carried o...
Article
All polymer organic solar cells afford unique potentials due to the tunable chemical and electronic properties of both polymer donors and polymer acceptors. Compared with the rapid development of polymer donors, the development of polymer acceptors lags far behind. To seek for high-performance polymer acceptors used in organic solar cells, based on...
Article
One of the most important aims in the development of high-energy materials is to improve their stability and thus ensure that they are safe to manufacture and transport. In this work, we theoretically investigated open-chain N4B2 isomers using density functional theory in order to find the best way of stabilizing nitrogen-rich molecules. The result...
Article
Upon application of heat or UV light, acyl azides undergo the Curtius rearrangement leading to an isocyanate with the loss of nitrogen gas, which is of great importance in organic chemistry and biological science. The mechanism of the thermal Curtius rearrangement has been made clear, but the photo-induced one remains controversial. In this work, t...
Article
The photophysical properties of tetraphenylethene (TPE) compounds may differ widely depending on the substitution pattern, for example with regard to the fluorescence quantum yield phi_f and the propensity to exhibit aggregation-induced emission (AIE). We report combined electronic structure calculations and nonadiabatic dynamics simulations to stu...
Article
A novel stable energetic compound (E)-1,2-diamino-1,2-dinitrodiboron (DANB) was theoretically designed based on the structure of 1,1-diamino-2,2-dinitroethene (FOX-7). Atomization method in combination with Hess' law was used to predict the heat of formation. The detonation velocity (D) and detonation pressure (P) of DANB were approximatively estim...
Article
Co-sensitization has been considered as a helpful strategy for improving the conversion efficiency in dye-sensitized solar cells (DSSCs). In this present, Zinc porphyrin dyes 1–4 have been designed based on SM315 which has achieved the record efficiency (13%). Simultaneously, these new dyes are anticipated to replace the previous dye XW11 which is...
Article
Understanding the photochemistry of organoboron compounds is essential to expand optoelectronic applications. In this work, the complete active space self-consistent field (CASSCF) and its second-order perturbation (CASPT2) methods combining with density functional theory (DFT) have been employed to investigate the elimination mechanisms of compoun...
Article
Full-text available
5-Diazo Meldrum's acid (DMA) undergoes a photo-induced Wolff rearrangement (WR). Recent gas-phase experiments have identified three photochemical products formed in a sub-ps scale after irradiation, a carbene formed after nitrogen loss, a ketene formed after WR and a second carbene formed after nitrogen and CO elimination (A. Steinbacher, et al. Ph...
Article
Electron-rich and electron-poor BN-heterocycles with benzyl-pyridyl chelate backbones and two bulky aryl groups on the boron center (Ar = tipp, BN-1; Ar = MesF, BN-2) have been found to display distinct molecular transformations upon irradiation by UV light. BN-1 undergoes an exceptionally efficient photoelimination reaction forming a BN-phenanthre...
Article
In this work, we report on the design and full prediction of four poly-nitro cage compounds, octanitrooctaprismane (ONOP), octanitrooctaazaprismane (ONOAP), tetranitrooctaprismane (TNOP), and tetranitrooctaazaprismane (TNOAP) at the B3LYP/6-31G (d,p) level using density functional theory (DFT). The results show that all compounds possess large posi...
Article
Full-text available
Organic-inorganic methylammonium lead halide perovskites have recently attracted great interest emerging as promising photovoltaic materials with a high 20.8% efficiency, but lead pollution is still a problem that may hinder the development and wide spread of MAPbI3 perovskites. To reduce the use of lead, we investigated the structures, electronic...
Article
Full-text available
Density functional theory calculations were used to study energetic and stability properties for a series of pentaprismane (C10H10) derivatives with different substituent groups (NO2, NO, CN, N3, NH2, NHNO2, and ONO2). The results indicated that the N3 and CN groups greatly increase while the ONO2 group decreases the heats of formation. Moreover, t...
Article
Perovskite solar cells (PSCs) with organic small molecules as hole transport materials (HTMs) have attracted considerable attention due to power conversion efficiencies as high as 20%. In the present work, three new spiro-type hole transport materials with spiro-core, i.e Spiro-F1, Spiro-F2, and Spiro-F3, are investigated by using density functiona...
Article
The mechanism behind aggregation induced emission (AIE) in the prototypical dimethyl tetraphenylsilole (DMTPS) molecule is investigated with ab initio calculations combining the CASSCF and CASPT2 methods with time-dependent DFT. DMTPS is AIE-active because it is strongly fluorescent in the aggregate phase but only weakly in solution. Based on the r...
Article
Full-text available
In recent years, perovskite solar cells have been considerably developed, however the lead in the absorber MAPbI3 is a potential threat to the environment. To explore potential alternatives, the structural and electronic properties of MAGeX3 (X = Cl, Br, I) were investigated using different density functional theory methods, including GGA-PBE, PBE-...
Article
The regeneration of ruthenium(II) dyes by cobalt redox mediator in dye-sensitized solar cells (DSSCs) has been investigated using density functional theory combined with the Marcus theory of electron transfer. Our results show that the regeneration reaction rates gradually increase with the growth of the dye protonation degree. By comparing the nat...
Article
We have performed a theoretical investigation using a combination of DFT/TDDFT and molecular dynamics simulations to explain the relationship between bulky donor groups and higher efficiencies for a recent indoline sensitizer YA422 derived from its counterparts IQ4 and YA421, which features an extended donor subunit for use in dye-sensitizer solar...
Article
NHC-B,N-heterocyclic compounds have been found to act as convenient precursors for obtaining either 1,3-azaborinine or 1H-imidazo[1,2-a]indole derivatives, which are two different and rare classes of compounds. The formation of these two classes of compounds from the NHC-B,N-heterocycles is highly selective depending on the external stimuli employe...
Article
For novel high-energy low-sensitivity energetic materials, a series of novel cycloalkanes derivatives Cm(N–NO2)m (m=3-8) were theoretically designed by substitution of the hydrogen atoms with N−NO2 group. Density functional theory (DFT) calculations in combination with the isodesmic reaction and the Kamlet−Jacobs equations were employed to predict...
Article
Full-text available
D-A-π-A-featured organic dyes incorporating diphenylquinoxaline unit (such as IQ4) have shown great potential in anti-aggregation and broaden spectral response in the field of dye-sensitized solar cells (DSSCs). The crucial restriction for quinoxaline-based cell to attain higher efficiency is the relatively low photocurrent density (JSC). In the pr...
Article
The regeneration processes of triphenylamine (TPA)-based dyes with cobalt redox mediator in dye-sensitized solar cells (DSSCs) have been investigated using density functional theory combined with the Marcus theory of electron transfer. Our results show that with the extension or rigidification of the oligothiophene conjugation linker the absorption...
Article
Combining density functional theory (DFT), time-dependent DFT, and density functional tight binding (DFTB) methods, we present a computational investigation on the aggregation effects of two organic dyes, WS-2 and WS-6, which are used as sensitizers in dye sensitized solar cells (DSSCs). The calculated absorption and emission spectra in solution an...
Article
Designed with electron-rich and electron-deficient groups as π-linkers, a series of novel unsymmetrical squaraine dyes (SQ) for dye-sensitized solar cells (DSSCs) have been simulated using density functional theory (DFT) and time-dependent DFT (TDDFT) methods. Dye/TiO2 complexes were also calculated to explore various properties on the interface. T...
Article
Full-text available
The structural and electronic properties of an organic dye C258 adsorbed onto the TiO2 (101) surface with two adsorption modes, monodentate (Mha) and bidentate bridging (BBH), have been investigated by using the density functional tight binding (DFTB) method. A detailed analysis of the adsorbate contributions of the dye molecule to band states of T...
Article
Density functional theory (DFT) calculations were carried out to explore the effects of chemically modifying the polypyridine ligands and design efficient Co-based redox mediators for dye-sensitized solar cells (DSSCs). Our results showed that the redox properties of cobalt complexes can be well tuned by altering the number and position of nitrogen...
Article
Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations have been carried out on the electronic structure and optical properties of a set of heterocycle-fused zinc porphyrazine (ZnPz) derivatives, aiming at screening efficient sensitizers for dye-sensitized solar cells (DSSCs). Our results show that the absorption spectra of the...
Article
Silicon is the leading semiconductor material in microelectronic industry. Owing to the large surface to volume ratio, low-dimensional Si nanostructures, for instance, silicon quantum dots exhibit diverse electronic and optical properties. Passivating the surface of Si nanostructures by a suitable species is thereby required to stabilize and engine...
Article
By means of density functional theory calculations, the adsorption process of I2 at Pt (111) surface in dye-sensitized solar cells (DSSCs) has been investigated. The obtained adsorption energies and stable structures depending on the adsorption sites of the Pt surface are in good agreement with experimental values. Our results show that the dissoci...

Citations

... The results from the abovementioned studies indicate that a decrease in the density of hydroxide groups on the ZnO surface and the modification of the surface Lewis acidity of ZnO can alleviate the instability at the ZnO/ CH 3 NH 3 PbI 3 interface and energy loss. Recently, Zhang et al. [41] demonstrated that passivation by the Lewis base molecule, 2-mercaptopyridine (2-MP), can increase the stability of CH 3 NH 3 PbI 3 . Hence, it can be considered that the fluorination of ZnO surfaces can increase the efficiency and stability of perovskite solar cells. ...
... NFAs possess distinct advantages on high-lying energy levels, strong and broad absorption in the visible region, appropriate phase separation for exciton dissociation, and efficient charge separation with low voltage loss [7,8]. Further improving the photoelectric properties of NFAs is of significance to prompt the PCEs of NFAs -based OSCs [9], such as extending sunlight absorption in the long-wavelength region and reducing the voltage loss during charge separation and transfer. Moreover, ternary polymer solar cells (PSCs) which consist of two donors or two acceptors can exhibit higher PCEs than binary ones. ...
... Thus, understanding the impact of end groups on the electronic and optical properties is helpful in tuning optical absorption, excited states properties, and performance of OSCs. The energy of LUMO is calculated by adding the energy of HOMO and the lowest excited state energy, as suggested by Yang et al. (2020). Before we compare the energy levels of newly designed NFAs, we have compared the HOMO and LUMO energy levels of ITIC with three different functionals such as meta-hybrid M05, long-range corrected CAM-B3LYP, ωB97XD, and N12 functionals. ...
... Similarly, cyclometallation of the N^C ligands also quenched the photoisomerization process of the B(ppy)Mes2 chromophore [40]. Several other studies have been carried out to obtain an in-depth knowledge of such chromophores and more can be found in references [38,[41][42][43][44][45][46]. Through various structural modifications and analogues, it has been established that photoisomerization could also be extended to N^C-chelate in addition to the ppy systems [47]. ...
... They also modeled optimized structures and binding energies of the ETM on the PbI 2 -terminated MAPbI 3 (110) interface, which showed that the additional N/Pb interface interaction between the nitrogen atoms in the ETMs and the lead atom in MAPbI 3 leads to stronger binding energies and easier electron injection (Figure 9c). 183 Similarly, Cao et al. reported a new series of hydrophilic fullerene derivatives, C70-DPM-OE, C70-(DPM-OE)2, C60-DPM-OE, and C60-(DPM-OE)2, with each phenyl group of the diphenylmethanofullerene (DPM) moiety decorated by an oligoether (OE) side group. A high PCE of 16% was achieved by applying the monoadduct fullerene derivative C70-DPM-OE as the ETL of the device, which was over 23% higher than their reference devices with PC71BM as ETM. ...
... Similarly, cyclometallation of the N^C ligands also quenched the photoisomerization process of the B(ppy)Mes2 chromophore [40]. Several other studies have been carried out to obtain an in-depth knowledge of such chromophores and more can be found in references [38,[41][42][43][44][45][46]. Through various structural modifications and analogues, it has been established that photoisomerization could also be extended to N^C-chelate in addition to the ppy systems [47]. ...
... Thus, we have considered the mPW1PW91 functional to evaluate the frontier energy values for both linear and cyclic molecules. HOMO, LUMO, and the difference between HOMO and LUMO energies (E g ) are the important factors that influence the optoelectronic properties and charge carrier transport properties of π-conjugated materials 20,36,37 . The pictorial representation of HOMO and LUMO wavefunctions obtained at the mPW1PW91/6-31G** level of theory for cyclic (C[PT] 12 4 ) molecules are depicted in Fig. 3. ...
... 64 Bai et al. synthesized GCN penel (CN nanoplatelets with the thickness of 12 nm) through vapor deposition polymerization, and then deposited (111)-oriented Au nanoparticles ($2 nm) on GCN (CN@Au (111)). 65 Interestingly, the VB of CN@Au (111)-60 (immersed in HAuCl 4 solution for 60 s) has downshifted by 0.46 eV compared with CN, indicating the larger driving force for water oxidation thermodynamically. In the CN@Au (111), the CN and Au nanoparticles maintained close contact, which promotes charge transfer and inhibits their recombination (photocurrent is 63 times that of CN). ...
... They also showed that the thiazole ring with an N-atom substituted at the b-position was more favourable for electron transport as compared to the a-substituted analogues. 29 Apparently, the electronic and charge transport properties of the nitrogen containing OSCs are found to be superior compared to their undoped counterparts. Furthermore, the aza-substituted organic radicals are thermodynamically more stable due to the strong electronegativity of the N-atom in the carbon matrix. ...
... Aside from the direct use of base-stabilized boriranes in materials science, these high energy species can also be used as reactive intermediates in the facile preparation of functional materials such as singly annulated borepins [56] and chiral N,B,X-heterocycles (X = S or O) [57]. Borepins are charge neutral, boron-containing analogues of the tropylium cation, where the boron atom is typically protected by bulky substituents [58]. ...