Nonradiative Electron-hole Recombination Research Articles

Compression of Organic Molecules Coupled with Hydrogen Bonding Extends the Charge Carrier Lifetime in BA2SnI4.

Two-dimensional (2D) metal halide perovskites, such as BA2SnI4 (BA═CH3(CH2)3NH3), exhibit an enhanced charge carrier lifetime in experiments under strain. Experiments suggest that significant compression of the BA molecule, rather than of the inorganic lattice, contributes to this enhancement. To elucidate the underlying physical mechanism, we apply a moderate compressive strain to the entire system and subsequently introduce significant compression to the BA molecules. We then perform ab initio nonadiabatic molecular dynamics simulations of nonradiative electron-hole recombination. We observe that the overall lattice compression reduces atomic motions and decreases nonadiabatic coupling, thereby delaying electron-hole recombination. Additionally, compression of the BA molecules enhances hydrogen bonding between the BA molecules and iodine atoms, which lengthens the Sn-I bonds, distorts the [SnI6]4- octahedra, and suppresses atomic motions further, thus reducing nonadiabatic coupling. Also, the elongated Sn-I bonds and weakened antibonding interactions increase the band gap. Altogether, the compression delays the nonradiative electron-hole recombination by more than a factor of 3. Our simulations provide new and valuable physical insights into how compressive strain, accommodated primarily by the organic ligands, positively influences the optoelectronic properties of 2D layered halide perovskites, offering a promising pathway for further performance improvements.

Graphene Quantum Dots as Hole Extraction and Transfer Layer Empowering Solar Water Splitting of Catalyst-Coupled Zinc Ferrite Nanorods.

Despite the narrow band gap energy, the performance of zinc ferrite (ZnFe2O4) as a photoharvester for solar-driven water splitting is significantly hindered due to its sluggish charge transfer and severe charge recombination. This work reports the fabrication of a hybrid nanostructured hydrogenated ZnFe2O4 (ZFO) photoanode with enhanced photoelectrochemical water-oxidation activity through coupling N-doped graphene quantum dots (GQDs) as a hole transfer layer and Co-Pi as a catalyst. The GQDs not only reduce the surface-mediated nonradiative electron-hole pair recombination but also induce a built-in interfacial electric field leading to a favorable band alignment at the ZFO/GQDs interface, helping rapid photogenerated hole separation and serving as a conducting hole transfer highway, improve the hole transportation into the Co-Pi catalyst for enhanced water oxidation reaction kinetics. The optimized ZFO/GQD/Co-Pi hybrid photoanode delivers a 23-fold photocurrent enhancement at 1.23 V versus the reversible hydrogen electrode (RHE) and a significant 360 mV reduction in the onset potential, reaching 0.65 VRHE compared with the ZFO photoanode under 1 sun illumination in a neutral electrolytic environment. This investigation underscores the mechanism of synergistic interplay between the hole transport layer and cocatalyst in boosting the solar-illuminated water-splitting activity of the ZFO photoanode.

Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride.

Poly(triazine imide)·Li+Cl- (PTI/Li+Cl-) as one of the most reported crystalline carbon nitrides has shown exciting potential for photocatalysis. However, understanding the role of Li+/Cl- in the photoexcited charge transfer in the time and space of PTI is a challenging problem. Here, we have investigated the nonradiative charge recombination of series ion intercalated PTI systems (PTI/Li+X-, where X = F, Cl, Br, and I) by performing the ab initio nonadiabatic molecular dynamics simulations. The results indicate that the intercalated anions in PTI/Li+Cl- and PTI/Li+Br- have the potential to trap holes, separate the electrons and holes, and prolong the nonradiative electron-hole recombination. In particular, ∼70% of holes in PTI/Li+Cl- can transport among interlayers toward the {0001} planes, while most of the electrons are transferred to the {101̅0} planes, exhibiting different transport pathways and directions. Furthermore, PTI/Li+Cl- has an electron-hole recombination time as long as 136 ns, which explains its excellent optoelectronic properties. This work provides a theoretical baseline for the reported facet engineering improvement of crystalline carbon nitride for overall water splitting.

Enhanced Nonradiative Charge Recombination in Microfiber-Based Bismuthene.

After the first report of a graphene-based passive mode-locking ultrafast fiber laser, two-dimensional materials as efficient saturable absorbers offer a new horizon in ultrafast fiber laser. However, the interactions on atomic scale between these two-dimensional materials and fiber and the fiber effect on the carrier dynamics have not been realized. To figure out the exact role of fiber and the carrier dynamics affected by the fiber substrate related to ultrafast photonics, bismuthene, a newly reported 2D quantum material used in a passive mode-locking fiber laser, deposited on α-quartz has been investigated. We surprisingly found that the α-quartz substrate can strongly accelerate the nonradiative electron-hole recombination of bismuthene in theory, and the transient absorption spectra of bismuthene on normal glass and α-quartz further verify the substrate effect on carrier dynamics of bismuthene. The discovery provides new thinking about substrate effect to regulate the performance of ultrafast mode-locking fiber lasers as well as ultrafast photonics.

Impact of large A-site cations on electron-vibrational interactions in 2D halide perovskites: Ab initio quantum dynamics.

Using abinitio nonadiabatic molecular dynamics, we study the effect of large A-site cations on nonradiative electron-hole recombination in two-dimensional Ruddlesden-Popper perovskites HA2APb2I7, HA = n-hexylammonium, A = methylammonium (MA), or guanidinium (GA). The steric hindrance created by large GA cations distorts and stiffens the inorganic Pb-I lattice, reduces thermal structural fluctuations, and maintains the delocalization of electrons and holes at ambient and elevated temperatures. The delocalized charges interact more strongly in the GA system than in the MA system, and the charge recombination is accelerated. In contrast, replacement of only some MA cations with GA enhances disorder and increases charge lifetime, as seen in three-dimensional perovskites. This study highlights the key influence of structural fluctuations and disorder on the properties of charge carriers in metal halide perovskites, providing guidance for tuning materials' optoelectronic performance.

Electron-Phonon Coupling-Mediated Ultralong Carrier Lifetime in an All-Inorganic Two-Dimensional Cs2PbI2Cl2 Perovskite: Explanation for the High Antisite Defect Tolerance.

Two-dimensional (2D) halide perovskite are appealing candidates for applications in optoelectronics and photovoltaics, but their energy conversion efficiency is severely limited by nonradiative electron-hole recombination. In most investigations, point defects with deep defect levels and deep charge-state transition levels in the band gap are treated as the carrier recombination centers. For the all-inorganic 2D Css 2PbI2Cl2, the IPb antisite defect is the most likely to form and cause nonradiative electron-hole recombination. By using density functional theory and ab initio nonradiative molecular dynamics calculations, we found that the IPb defect can introduce the deep acceptor and donor levels into the band gap. Because electron-phonon coupling gives rise to weak nonadiabatic coupling and rapid loss of electronic coherence, those levels lead to a reduction of the carrier loss and the prolongation of the excited-state carrier lifetime, thereby enhancing the photoelectric and defect tolerance properties of the Cs2PbI2Cl2 material. These results could deepen the understanding of the chemistry of defects and carrier dynamics in perovskite materials.

Nonadiabatic molecular dynamics study on effect of Ge/Sn alloy on hot carrier relaxation of CsPbBr<sub>3</sub> perovskite

Perovskite solar cells have been a prominent focus in the field of photovoltaics in recent decades, owing to their exceptional performance: easy synthesis, and cost-effectiveness. The all-inorganic cesium-based perovskite CsPbBr<sub>3</sub>, known for its remarkable thermal stability, has become a star material in the field of optoelectronics due to its outstanding luminescent properties. Despite the high efficiency of lead-based perovskite solar cells, the toxicity associated with lead and the poor long-term stability of these devices remain significant barriers to their large-scale commercialization. As is well known, non-radiative electron-hole recombination significantly shortens the carrier lifetime, acting as a primary pathway for excited state charge to loss energy. This phenomenon directly affects the photovoltaic conversion efficiency and charge transfer performance of perovskite materials. Therefore, maximizing the reduction of non-radiative recombination energy loss in perovskite solar cells has become a crucial research focus. In this study, a systematic exploration is conducted by using a non-adiabatic molecular dynamics approach combined with time-dependent density functional theory to investigate the excited-state carrier dynamics of CsPbBr<sub>3</sub> and its alloyed structures, CsPb<sub>0.75</sub>Ge<sub>0.25</sub>Br<sub>3</sub> and CsPb<sub>0.5</sub>Ge<sub>0.25</sub>Sn<sub>0.25</sub>Br<sub>3</sub>. The study comprehensively analyzes the non-radiative electron-hole recombination scenarios and the mechanisms for reducing charge energy loss based on crystal structure, electronic properties, and excited-state properties. The research findings reveal that alloying with Sn/Ge can reduce the bandgap, increase non-adiabatic coupling, and shorten the decoherence time. The interplay of reduced quantum decoherence, smaller bandgap, and larger non-adiabatic coupling effectively decelerates the electron-hole recombination process. Consequently, the carrier lifetime of the CsPb<sub>0.75</sub>Ge<sub>0.25</sub>Br<sub>3</sub> system extends by 1.6 times. Moreover, under the joint influence of Sn/Ge, the carrier lifetime of the CsPb<sub>0.5</sub>Ge<sub>0.25</sub>Sn<sub>0.25</sub>Br<sub>3</sub> system extends by 4.2 times compared with those of the original system. The overall sequence follows CsPb<sub>0.5</sub>Ge<sub>0.25</sub>Sn<sub>0.25</sub>Br<sub>3</sub> > CsPb<sub>0.75</sub>Ge<sub>0.25</sub>Br<sub>3</sub> > CsPbBr<sub>3</sub>. This study underscores the significant influence of binary alloying of B-site metal cations (in the perovskite structure <i>ABX</i><sub>3</sub>, where B-site refers to the metal cation) on the non-radiative electron-hole recombination of CsPbBr<sub>3</sub>.This research presents an effective alloying scheme that substantially prolongs the carrier lifetime of perovskites, offering a rational approach to optimizing solar cell performance. It lays the groundwork for the future design of perovskite solar cell materials.

Resolving the Puzzle of Charge Carrier Lifetime in ZnO by Revisiting the Role of Oxygen Vacancy.

Zinc oxide (ZnO) is a wide bandgap prototypical n-type semiconductor due to the presence of intrinsic oxygen vacancies (VO). The VO can readily transfer to the most energetically favorable +2 charged VO (VO2+) by losing two electrons mediated by the metastable VO1+ defect. Nevertheless, the influence of charged VO on the charge dynamics in ZnO and the underlying mechanisms remain elusive. By performing nonadiabatic molecular dynamics simulations of the charge trapping and recombination processes, we show that both VO1+ and VO2+ slow down the nonradiative electron-hole recombination via assisted defect states and, thus, extending charge carrier lifetime compared to pristine ZnO. Our study contributes to identifying the different recombination pathways that take place in VO1+ and VO2+ of n-type ZnO systems, providing useful guidance for designing high-performance ZnO-based devices.

Ab Initio Quantum Dynamics Simulation of the Impact of Graphene on the Carrier Lifetime of the ZnV2O6 Photocatalyst.

We used a nonadiabatic molecular dynamics simulation to determine the carrier dynamics of a graphene/ZnV2O6 heterostructure in the search for an effective photocatalyst material. The C-2p orbital promotes the wave function overlap, guiding electrons to move between graphene and ZnV2O6, successfully achieving good mixing with the valence and conduction bands in ZnV2O6 materials, which is conducive to supporting carrier migration. The overlap between graphene/ZnV2O6 electrons and hole wave functions is less than that of ZnV2O6, and there is small absolute nonadiabatic coupling. The charge separation caused by graphene increases the carrier lifetime and prevents nonradiative electron-hole recombination. This study reveals the microscopic mechanism of extending the carrier lifetime of ZnV2O6 by introducing graphene, providing useful insights for regulating the electronic structure, promoting electron transfer and ultrafast electron and hole transfer. This strategy provides design considerations for advanced photocatalytic materials.

Tensile Strain-Dependent Ultrafast Electron Transfer and Relaxation Dynamics in Flexible WSe2/MoS2 Heterostructures.

Understanding and controlling carrier dynamics in two-dimensional (2D) van der Waals heterostructures through strain are crucial for their flexible applications. Here, femtosecond transient absorption spectroscopy is employed to elucidate the interlayer electron transfer and relaxation dynamics under external tensile strains in a WSe2/MoS2 heterostructure. The results show that a modest ∼1% tensile strain can significantly alter the lifetimes of electron transfer and nonradiative electron-hole recombination by >30%. Ab initio non-adiabatic molecular dynamics simulations suggest that tensile strain weakens the electron-phonon coupling, thereby suppressing the transfer and recombination dynamics. Theoretical predictions indicate that strain-induced energy difference increases along the electron transfer path could contribute to the prolongation of the transfer lifetime. A subpicosecond decay process, related to hot-electron cooling, remains almost unaffected by strain. This study demonstrates the potential of tuning interlayer carrier dynamics through external strains, offering insights into flexible optoelectronic device design with 2D materials.

Great Influence of Pressure and Isotope Effects on Nonradiative Charge Loss in Hybrid Organic-Inorganic Perovskites.

The intrinsic softness of hybrid organic-inorganic perovskites (HOIPs) allows their lattice and optoelectronic performance to be tunable to external pressure. Using nonadiabatic (NA) molecular dynamics, we demonstrate that a mild pressure accelerates hot electron relaxation and suppresses nonradiative electron-hole recombination in CH3NH3PbI3. Both processes are governed by NA coupling, which is enhanced between the electronic states of the quasi-continuous bands while is decreased between the band-edge states by reducing the electron-hole wave function overlap. Hydrogen/deuterium isotope exchange alleviates the pressure-induced NA coupling by increasing lattice rigidity and decreasing wave function overlap, slowing down both the hot electron relaxation and electron-hole recombination processes. The simulated time scales of sub-3 ps for hot electron relaxation and half nanoseconds for recombination agree well with the experiments. The study suggests that the isotope exchange can mitigate the pressure-caused fast losses of hot electrons and further prolong the charge carrier lifetime in HOIPs.

Nuclear Quantum Effects Prolong Charge Carrier Lifetimes in Hybrid Organic-Inorganic Perovskites.

Hybrid organic-inorganic perovskites (HOIPs) contain light hydrogen atoms that exhibit significant nuclear quantum effects (NQEs). We demonstrate that NQEs have a strong effect on HOIP geometry and electron-vibrational dynamics at both low and ambient temperatures, even though charges in HOIPs reside on heavy elements. By combining ring-polymer molecular dynamics (MD) and ab initio MD with nonadiabatic MD and time-dependent density functional theory and focusing on the most studied tetragonal CH3NH3PbI3, we show that NQEs increase the disorder and thermal fluctuations through coupling of the light inorganic cations to the heavy inorganic lattice. The additional disorder induces charge localization and decreases electron-hole interactions. As a result, the nonradiative carrier lifetimes are extended by a factor of 3 at 160 K and 1/3 at 330 K. The radiative lifetimes are increased by 40% at both temperatures. The fundamental band gap decreases by 0.10 and 0.03 eV at 160 and 330 K, respectively. By enhancing atomic motions and introducing new vibrational modes, NQEs strengthen electron-vibrational interactions. Decoherence, determined by elastic scattering, accelerates almost by a factor of 2 due to NQEs. However, the nonadiabatic coupling, driving nonradiative electron-hole recombination, decreases because it is more sensitive to structural distortions than atomic motions in HOIPs. This study demonstrates, for the first time, that NQEs should be considered to achieve an accurate understanding of geometry evolution and charge carrier dynamics in HOIPs and provides important fundamental insights for the design of HOIPs and related materials for optoelectronic applications.

Investigating of the anticancer activity of salen/salophen metal complexes based on graphene quantum dots: Induction of apoptosis as part of biological activity

This research work is the first report on the synthesis and stabilization of [Fe-Salophen] and [Fe-Salen] complexes by two methods of surface modification and anchoring of synthesized Schiff base ligand on the surface of graphene quantum dots (GQDs). The GQDs contain oxygenated functional groups that can act as non-radiative electron-hole recombination centers. Therefore removing these oxygen functional groups may improve quantum yield by reducing or deactivating the surface. In this work, GQDs with the amine functional group were synthesized with a quantum yield of 37.48%. The physicochemical properties of GQDs were investigated by Ultraviolet–visible (UV–Vis) and fluorescence spectroscopies, Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), Powder X-ray diffraction (PXRD), Transmission electron microscope (TEM). The synthesis of GQDs-[Fe-Salen] and GQDs-[Fe-Salophen] was evaluated by FT-IR, Inductively coupled plasma atomic emission spectroscopy (ICP-AES) and Energy dispersive X-Ray analysis (EDX) analyses. Then, using MTT- assay, annexin V-FITC/PI, DAPI staining and cellular uptake assays, the biochemical activity of these complexes on the MCF7 cell line was investigated. The results shows that GQDs-[Fe-Salen] and GQDs-[Fe-Salophen] affect the survival of MCF7 cancer cells and, by nuclear fragmentation cause 35.77% and 19.41% of early apoptosis in cells, respectively. Also was found cellular uptake of GQDs-[Fe-Salen] is higher than that of GQDs-[Fe-Salophen].

Tunable nonradiative recombination dynamics and charge injection of graphene quantum dots for energy conversion applications by controllable functionalization

Understanding the dependence of optoelectronic properties and charge transfer processes on the specified functionalization pattern of the graphene quantum dot (GQD) surface is key to deciphering the photovoltaic and photocatalytic mechanisms. In the present work, the photophysical properties and energy conversion efficiency of OCH3-functionalized GQDs are investigated using first-principle calculations. Furthermore, the nonradiative electron–hole recombination dynamics is analyzed using Fermi’s golden rule. Our results show that the OCH3 group has different binding energies on the GQD surface depending on its binding configuration and forms different oxidation patterns of the GQD controlled by the reaction temperature. Both basal and edge oxidation reduce the bandgaps of GQDs due to the electron localization effect, resulting in differing chemical stability. In addition, basal oxidation provides more degrees of freedom with which to tune the wavelengths and oscillator strengths of the low absorption peaks. Although edge oxidation provides a stronger electron-injection driving force from the GQDs into the TiO2 and facilitates charge separation, it also leads to faster nonradiative recombination, which reduces charge separation. Overall, our work reveals a detailed mechanistic picture of energy conversion in oxidized GQDs.

Spin–Orbit Coupling Notably Retards Non-radiative Electron–Hole Recombination in Methylammonium Lead Triiodide Perovskites

The giant spin-orbit coupling (SOC) of a heavy lead element significantly extends charge carrier lifetimes of lead halide perovskites (LHPs). The physical mechanism remains unclear and requires a quantum dynamics perspective. Taking methylammonium lead iodide (MAPbI3) as a prototypical system and using non-adiabatic molecular dynamics combined with 1/2 electron correction, we show that SOC notably reduces the non-radiative electron-hole (e-h) recombination by decreasing the non-adiabatic coupling (NAC) primarily as a result of SOC decreasing the e-h wave function overlap by reshaping the electron and hole wave functions. Second, SOC causes spin mismatch subject to spin-mixed states, which further decreases NAC. The charge carrier lifetime is about 3-fold longer in the present of SOC relative to the absence of SOC. Our study generates the fundamental understanding of SOC minimizing non-radiative charge and energy losses in LHPs.

Boosting photocatalytic Cr(VI) reduction activities of layered COF through regulating donor-acceptor units and the orientation of imine bonds

In this work, three isoreticular covalent-organic frameworks (COFs) were successfully synthesized at room temperature, namely C1, C2, and C3, respectively. Due to their wide absorption ranges and sufficient photoredox potentials, the constructed COFs exhibited good photocatalytic performance for reducing Cr(VI). Among them, C2 displayed the best photocatalytic performance, which may be attributed to the unique donor-acceptor structure, good light absorption, and excellent photoinduced carriers’ separation and migration efficiency. When the COFs were modified with gold nanoparticles (labeled as Au@C1, Au@C2, and Au@C3), their photocatalytic performance can be further improved. For Au@C2, 98.2% of Cr(VI) can be reduced within 120 min, and its photocatalytic activity can be maintained over five reaction cycles. The structure-activity correlation was studied via both experimental and DFT calculation methods. It is shown that although C3 displayed wider absorption range and smaller energy band gap, its photocatalytic activity was much lower than C2. This may be due to the rapid nonradiative electron-hole recombination in C3, leading to low light utilization. These results indicate that to construct excellent COF photocatalysts, it not only needs to pursue wider absorption range and smaller energy band gap, but also improve the utilization of light energy and photogenerated charge carriers. In addition, the active species and photocatalytic mechanism were also studied.

Improved Defect Tolerance and Charge Carrier Lifetime in Tin-Lead Mixed Perovskites: Ab Initio Quantum Dynamics.

Simulations by nonadiabatic (NA) molecular dynamics demonstrate that mixing tin with lead in CH3NH3PbI3 can passivate the midgap state created by an interstitial iodine (Ii) via the imposed compressive strain and upshifted valence band maximum, reduce NA coupling by decreasing electron-hole wave functions overlap, and shortens pure-dephasing time by introducing high-frequency phonon modes. Thus, the charge carrier lifetime extends to 3.6 ns due to the significantly reduced nonradiative electron-hole recombination, which is an order of magnitude longer than the Ii-containing CH3NH3PbI3, over 2.5 times longer than the pristine CH3NH3PbI3 (1.4 ns), and even 1.7 times longer than the tin-lead mixed perovskite without the Ii defects (2.1 ns). Tin-lead alloying simultaneously increases the Ii defect formation energy to 0.402 eV from 0.179 eV in CH3NH3PbI3, which effectively enhances defect tolerance by reducing the defect concentration. The study reveals the factors controlling the enhanced performance of tin-lead mixed perovskite solar cells.

Interlayer Doping of Cu on Bilayer Black Phosphorus for Enhanced Charge Transfer and Transport Properties.

Metal doping between black phosphorus (BP) layers has great advantages in modulating electronic properties. Here, the effects of Cu intercalation on charge transfer and carrier dynamics are investigated by theoretical calculations. Relative to the pristine bilayer BP, Cu suppresses the nonradiative electron-hole recombination, reducing the major pathways of energy and current loss. Furthermore, we investigate a novel pn homogeneous junction based on the Cu-doped bilayer BP, which shows enhanced transport properties and Ohmic contact characteristics. This is because doping leads to the transformation of BP from p-type to n-type, charge accumulation on conduction bands allows electrons to be easily transferred to the p-type bilayer BP, and associated electrical properties can be modulated by the doping concentration. This study has fundamental importance for understanding structure-property relationships in metal intercalation, which is an important guidance for integration and interlayer engineering for two-dimensional materials.

Anion Doping Delays Nonradiative Electron-Hole Recombination in Cs-Based All-Inorganic Perovskites: Time Domain ab Initio Analysis.

Using time-domain density functional theory combined with nonadiabatic (NA) molecular dynamics, we demonstrate that composition engineering of the X-site anions has a strong influence on the nonradiative electron-hole recombination and thermodynamic stability of cesium-based all-inorganic perovskites. Partial substitution of iodine(I) with bromine (Br) and acetate (Ac) anions reduces the NA electron-vibrational coupling by minimizing the overlap between the electron and hole wave functions and suppressing atomic fluctuations. The doping also widens the energy gap to further reduce the NA coupling and to enhance the open-circuit voltage of perovskite solar cells. These factors increase the charge carrier lifetime by an order of magnitude and improve structural stability in the series CsPbI1.88BrAc0.12 > CsPbI2Br > CsPbI3. The fundamental atomistic insights into the influence of anion doping on the photophysical properties of the all-inorganic lead halide perovskites guide the design of efficient optoelectronic materials.

Sulfur-Vacancy Passivation via Selenium Doping in Sb2S3 Solar Cells: Density Functional Theory Analysis

Antimony sulfide (Sb2S3) has attracted great attention during the past few decades as a light-harvesting material for solar cells owing to its earth abundance and low toxicity. Meanwhile, various point defects limit the efficiency improvement below the power conversion efficiency (PCE) of 10%, especially for S vacancy defects with lower defect formation energy. However, recent experiments have reported that Se doping has suppressed the density of defects and improved photoelectric performance in Sb2S3 solar cells. We adopt the first principles to simulate defect formation energies, charge localization, phonon spectrum, and defect migration dynamics for Sb2S3 structures, indicating that Se doping contributes to increasing the formation energy and inhibiting the formation of the sulfur vacancy defect. Meanwhile, the addition of Se also reduces the overlap between vibrational configurations in initial and final states, suppresses nonradiative electron–hole recombination, prolongs the minority carrier lifetime, and decreases charge and energy losses in Sb2S3 solar cells. The results contribute to the atomistic understanding of the properties of sulfur-vacancy passivation via Se doping and afford the design of high-performance optoelectronic materials.