Red-shifted Absorption Spectra Research Articles

First Principles Study of the Photoelectric Properties of Alkaline Earth Metal (Be/Mg/Ca/Sr/Ba)-Doped Monolayers of MoS2.

The energy band structure, density of states, and optical properties of monolayers of MoS2 doped with alkaline earth metals (Be/Mg/Ca/Sr/Ba) are systematically studied based on first principles. The results indicate that all the doped systems have a great potential to be formed and structurally stable. In comparison to monolayer MoS2, doping alkaline earth metals results in lattice distortions in the doped system. Therefore, the recombination of photogenerated hole-electron pairs is suppressed effectively. Simultaneously, the introduction of dopants reduces the band gap of the systems while creating impurity levels. Hence, the likelihood of electron transfer from the valence to the conduction band is enhanced, which means a reduction in the energy required for such a transfer. Moreover, doping monolayer MoS2 with alkaline earth metals increases the static dielectric constant and enhances its polarizability. Notably, the Sr-MoS2 system exhibits the highest value of static permittivity, demonstrating the strongest polarization capability. The doped systems exhibit a red-shifted absorption spectrum in the low-energy region. Consequently, the Be/Mg/Ca-MoS2 systems demonstrate superior visible absorption properties and a favorable band gap, indicating their potential as photo-catalysts for water splitting.

First‐Principles Study of the Effects of La2+/3+ Doping and Oxygen Vacancies on TiO2 Magnetism, Carrier Lifetime, Activity, and Absorption Spectra

The effects of photocatalytic performance and magnetism between La doping and oxygen vacancy on rutile and anatase TiO2 systems are rarely compared. Oxygen vacancies in rutile and anatase TiO2 are also experimentally challenging to control accurately. Herein, the first‐principles generalized gradient approximation (GGA + U) method is used to investigate the effects of La2+/La3+doping and oxygen vacancy on TiO2 magnetism and photocatalytic performance. Results of magnetic calculation show that La2+ doping and oxygen vacancies are magnetic to TiO2, whether rutile or anatase, and that the bound magnetic polaron is the source of ferromagnetism in the anatase Ti15La2+O31 system. The anatase Ti30La22+O62 system can achieve room‐temperature ferromagnetism at Curie temperature. The calculation results of photocatalytic performance show that the anatase‐type Ti15La3+O31 system has minimum formation energy, the highest stability, maximum electric dipole moment, the strongest carrier activity, the strongest polarization ability, the slowest electron–hole recombination, the longest lifetime, and remarkable absorption spectrum redshift among the tested systems.

Elucidating modelling of C≡N-based carbazole-arylamine hole transporting materials for efficient organic and perovskite solar cells

Recently, the scientific community has shown great interest in hole transport materials (HTMs) to develop efficient and stable organic and perovskite solar cells. To boost the photovoltaic performance of these solar cell devices, scientists have been investigating the use of modified HTMs. In this study, we have developed a distinctive and proficient approach to building a better photovoltaic material by modifying the endcaps of the reference (MA). Specifically, we designed five new efficient HTMs (MA1-MA5) through molecular engineering on a terminal of reference molecule MA. Using density functional theory (DFT) and time-dependent-DFT methods, we theoretically characterized the key characteristics of these newly designed materials, including the orientation of frontier molecular orbitals (FMO), absorption maxima, the partial density of states (PDOS), binding energies, reorganization energy, transition density matrix, fill factor (FF), open-circuit voltages (Voc) and power conversion efficiencies (PCEs) for these materials. Our theoretical representations revealed that newly constructed materials (MA1-MA5) have a highly red-shifted absorption spectrum with lower binding energies and narrow energy gaps, making them ideal for charge shifting. Among these designed MA1-MA5 materials, the MA1 has the potential to produce as much as higher 23.24% PCE when it will be used in fabricating solar cell devices, whereas, the other designed materials MA2-MA4 has also very comparable and much higher PCE values than the refence molecule MA. These findings demonstrate our efficient designing approach to tune the photovoltaic and optoelectronic properties of the HTMs, and we recommend these engineered materials for the future developments of an efficient solar cell devices.

Bridge molecule thiourea enforced polyaniline growing on activated carbon fiber for wearable braidable-supercapacitor

The bridge molecule thiourea (TU) enforced polyaniline (PANI) growing on activated carbon fiber (ACF) is applied to synthesize polyaniline-thiourea-activated carbon fiber (PANI-TU-ACF) through surface activation, hydrothermal treatment and electrochemical deposition processes for wearable braidable-supercapacitor. Experimental measurement and theoretical calculation demonstrate that PANI-TU-ACF involves amide bonding interface between ACF and TU and hydrogen bonding interface between TU and PANI, thus confirming the formation of bridging structure. The absorption spectrum red-shift of N–H vibration peak keeps in agreement with the declined bonding energy of N–H bond achieved by partial atom potential simulation calculation, which proves the formation of hydrogen bonding in PANI-TU-ACF. PANI-TU-ACF exhibits larger N(E) value and lower HOMO-LUMO energy gap than PANI-ACF, indicating its higher electrical conductivity. PANI-TU-PANI shows more lowered interface energy than PANI-ACF, suggesting its higher stability. PANI-TU-ACF electrode delivers excellent capacitance of 563.8F/g at 1 A/g and cycling stability of 89.1 % for 2000 cycles. Wearable braidable-supercapacitor based on PANI-TU-ACF electrode delivers energy density of 62.9 Wh kg−1 at power density of 800 W kg−1, maintains high capacitance retention of 90.13 % after 2000 charging/discharging cycles. The interfacial bonding strengthened PANI-TU-ACF with excellent performance displays potential in wearable supercapacitors.

Structure-Electrochemical Property Relationship of F vs 2F Substituents in Low Bandgap Conjugated Polymers

Two alternating copolymers bearing fluorinated benzothiadiazole as a strong acceptor unit and dithienopyrrole as a strong donor unit were designed and synthesized to discuss the effect of the number of fluorine atom substitution. The polymers were characterized via cyclic voltammetry, spectroelectrochemistry, electrochemical impedance spectroscopy and galvanostatic charge discharge studies. Besides a red shift in absorption spectra, an anodic shift was also observed in the oxidation potentials when number of fluorine atom increases in the polymer backbone. Galvanostatic charge-discharge (GCD) studies revealed that difluorinated polymer exhibited enhanced area specific capacitance compared to mono fluorinated polymer.

Hybrid of Conjugated Polymers with Incorporation of Metal Oxide Nanocomposites for Improving Optoelectronic Properties

Herein, the incorporation of TiO2 nanoparticles (NPs), SiO2 NPs, and their nanocomposite (STNC) to enhance the optoelectronic properties of the hybrid of poly[9,9′‐di‐n‐octylfluorenyl‐2,7‐diyl] (F8), poly[2‐methoxy‐5(2‐ethylhexyl)‐1,4‐phenylenevinylene)] (MEH‐PPV), and poly[2‐methoxy‐5‐(3,7‐dimethyl‐octyloxy)‐1,4‐phenylenevinylene]‐end capped with dimethylphenyl (MDMO–PPV–DMP) are revealed. The tune of the donor (F8) conjugated length can be detected from the red shift in absorption spectra when TiO2 NPs and SiO2 NPs are added, as well as an increase in emission intensity of the donor. The addition of acceptors (MEH–PPV or MDMO–PPV–DMP) to the donor results in a new absorption peak at 510 nm, which increases when TiO2 NPs and SiO2 NPs or STNC are incorporated into the ternary hybrid. The incorporation of STNC into F8 is anticipated to reduce the donor energy bandgap and improve the energy transfer from F8 to both acceptors. Moreover, Förster resonance energy transfer (FRET) is improved in the ternary hybrid, as evidenced by enhanced emission spectra of the donor and both acceptors, increased broadness of photoluminescence excitation spectra, and shifting blue color toward white region. The ternary hybrid with STNC‐based organic light‐emitting diode shows superior current and turn‐on voltage compared to other devices, which is likely due to its superior FRET.

Push–pull octaphenylporphyrins with mixed substituents pattern: Synthesis, redox, ultrafast dynamics and nonlinear optical studies

A new family of β-functionalized octaphenylporphyrins, MOPP(NO2)Br3 (M = 2H, ZnII, NiII, or CuII, and OPP = octaphenylporphyrin) has been synthesized possessing unsymmetrical substitutions of bromo and nitro groups and the effect of asymmetrical substitutions on the redox, spectral, ultrafast dynamics, and nonlinear optical properties of the porphyrin macrocycles are investigated. Routes for the mixed functionalized OPPs begin with the bromination of NiOPP(NO2), leading to the formation of NiOPP(NO2)Br3 and H2OPPBr4. These ‘push–pull’ OPPs exhibited nonplanar conformation, red-shift in absorption spectra, tunable redox properties, and very high ground state dipole moments due to nonplanarity and asymmetric β-substitutions. All synthesized porphyrins exhibited a bathochromic shift (λmax = 23–38 nm) in the B band and λmax = 21–83 nm in the last Q band in comparison to MOPP due to attachment of the bromo and nitro groups on its peripheral positions. In the cyclic voltammograms, the first oxidation and reduction potential showed an anodic shift compared to its parent porphyrins due to the presence of strong electron acceptor bromo and nitro groups, which are present on the porphyrin periphery. These β-functionalized octaphenylporphyrins have shown excellent nonlinear optical response. The observed structure-dependent nonlinear refractive index (n2) values are in the range of ∼ 0.37–1.68 × 10−19 m2 W−1, and two-photon absorption coefficient (β) values are in the range of ∼ 0.19–4.56 × 10−12 m W−1. The transient absorption studies reveal that the decay dynamics of ZnOPP(NO2)Br3 exhibited long-lived τ1 component, while NiOPP(NO2)Br3 exhibited long-lived τ2 component than other OPP derivatives.

Naphthaldehyde-Based Schiff Base Chemosensor for the Dual Sensing of Cu2+ and Ni2+ Ions.

In this study, a simple Schiff base sensor 1-(((4-nitrophenyl)imino)methyl)naphthalen-2-ol(NNM) has been used for chemosensing of metal ions. The metal sensing properties of sensor NNM have been investigated using UV-visible and fluorescence spectroscopic approaches. The spectral investigations revealed a red shift in absorption spectra and quenching in the emission band of the ligand molecule in the presence of Cu2+ and Ni2+ ions. The binding stoichiometry of sensor NNM for the analyte (Cu2+ and Ni2+ ions) has been investigated by the Job's plot analysis and found to be 1:1 (NNM:Analyte). The data of the Benesi-Hildebrand plot demonstrated that NNM detected Cu2+ and Ni2+ ions in nanomolar quantity. The binding insights among NNM and analytes (Cu2+ and Ni2+ ions) have been confirmed by shifted IR signals. Moreover, the reusabilty of the sensor has been investigated using an EDTA solution. In addition, the sensor NNM also successfully applied to real water samples for the identification and measurement of Cu2+ and Ni2+ ions. Hence, this system could be highly applicable in environmental and biological applications.

One, Two Three - Phosphaalkene Decoration Tailoring Solubility and Electronic Properties of Truxene-Based Electron Acceptors.

We report the functionalization and deplanarization of truxenes using pnictaalkene fragments. Selective introduction of one, two, or three Mes*-Pn fragments provides up to three fully reversible reductions based on the Pn=C fragments. The incorporation of the unsaturated heteroelement fragment as well as the contortion of the truxene core result in significantly red-shifted absorption spectra and interesting opto-electronic properties which are studied by electrochemistry and spectro-electrochemistry. Incorporation of arsaalkene (As=C) motifs gives significantly milder reduction potentials and red-shifted absorption, while phosphaalkene decorated truxene P3 can be functionalized using Au(I)Cl coordination. Furthermore, solubility is markedly increased upon incorporation of the Pn-Mes* fragments which renders these materials suitable for solution processing.

Effects of Halogenation on Cyclopentadithiophenevinylene-Based Acceptors with Excellent Responses in Binary Organic Solar Cells.

In recent years, non-fused non-fullerene acceptors (NFAs) have attracted increasing consideration due to several advantages, which include simple preparation, superior yield, and low cost. In the work reported here, we designed and synthesized three new NFAs with the same cyclopentadithiophenevinylene (CPDTV) trimer as the electron-donating unit and different terminal units (IC for FG10, IC-4F for FG8, and IC-4Cl for FG6). Both halogenated NFAs, i.e., FG6 and FG8, show red-shifted absorption spectra and higher electron mobilities (more pronounced for FG6) in comparison with FG10. Moreover, the dielectric constants of these materials also increased upon halogenation of the IC terminal units, thus leading to a reduction in the exciton binding energy, which is favorable for dissociation of excitons and subsequent charge transfer despite the driving force (highest occupied molecular orbital and lowest unoccupied molecular orbital offsets) being very small. The organic solar cells (OSCs) constructed using these acceptors and PBDB-T, as the donor, showed PCE values of 15.08, 12.56, and 9.04% for FG6, FG8, and FG10, respectively. The energy loss for the FG6-based device was the lowest (0.45 eV) of all the devices, and this may be attributed to it having the highest dielectric constant, which leads to a reduction in the binding energy of exciton and a small driving force for hole transfer from FG6 to PBDB-T. The results indicate that the NFA containing the CPDTV oligomer core and halogenated terminal units can efficiently spread the absorption spectrum to the NIR zone. Non-fused NFAs have a bright future in the quest to obtain efficient OSCs with low cost for marketable purposes.

Exploring structural, electronic, magnetic, and optical properties of CeO2-X (X = Pt/Ni) doped and Pt-Ni co-doped CeO2 for optoelectronic applications

Employing DFT technique, we perform Pt/Ni doping and Pt-Ni co-doping into CeO2. We study the structural, electronic, magnetic, and optical properties of CeO2 with selected dopants using Wien2k code. Spin-polarized DOS illustrate non-magnetic character of pure CeO2 while Pt/Ni/Pt-Ni doping yields magnetism into CeO2 with magnetic moment values of 2.2502 μ B, 2.5683 μ B, and 3.9190 μ B, respectively. Active participation of Ce 4f-, Pt 4d- and Ni 3d-states at the Fermi level suggests remarkable improvement in the conduction process. p-d hybridization is observed and it produces good response in electronic properties. Pt:CeO2 and Pt-Ni:CeO2 exhibit blueshift while Ni:CeO2 exhibit redshift in absorption spectrum. We notice an enhancement in optical absorption and conductivity with decreased reflectivity of these proposed materials in the UV region. Tuning of absorption spectra and decrease in band gap of these materials indicate their uses for photocatalytic, photonic, optoelectronics and power electronic devices.

Molecular modification effects on the electrochromic and photochromic properties of diarylethene with intramolecular isomerization behavior.

Diarylethene (DAE) is one of the most widely used functional units for electrochromic or photochromic materials. To better understand the molecular modification effects on the electrochromic and photochromic properties of DAE, two modification strategies, substitution with functional groups or heteroatoms, were investigated theoretically by density functional theory calculations. It is found that red-shifted absorption spectra caused by a decreased highest occupied molecular orbital-lowest unoccupied molecular orbital energy gap and S0 → S1 transition energy during the ring-closing reaction become more significant by adding different functional substituents. In addition, for two isomers, the energy gap and S0 → S1 transition energy decreased by heteroatom substitution of S atoms with O or NH, while they increased by replacing two S atoms with CH2. For intramolecular isomerization, one-electron excitation is the most effective way to trigger the closed-ring (O → C) reaction, while the open-ring (C → O) reaction occurs most readily in the presence of one-electron reduction. Moreover, it is confirmed that substitution with strong electron donating groups (-OCH3/-NH2) or with one O/two CH2 heteroatoms leads to a more favorable closed-ring (O → C) reaction. Functionalized with strong electron-withdrawing groups (-NO2 and -COOH) or one/two NH heteroatom substitutions, the open-ring (C → O) reaction is easier. Our results confirmed that the photochromic and electrochromic properties of DAE can be tuned effectively by molecular modifications, which provides theoretical guidance for the design of new DAE-based photochromic/electrochromic materials.

Selenium‐Based Nonfused Electron Acceptors for Efficient Organic Photovoltaic Cells

Selenium heterocycles are widely used in constructing organic semiconductors due to their advantages in narrowing the bandgap and enhancing the intermolecular packing. Herein, the application of Se substitution in designing nonfused electron acceptors (nfEAs) is studied. From a thiophene analog (A4T‐16), three nfEAs with two (ASe‐1 and ASe‐2) or four (ASe‐3) selenophene units are synthesized. The results suggest that the incorporation of Se atoms will downshift the lowest unoccupied molecular orbit level, upshift the highest occupied molecular orbit level, and exhibit redshifted absorption spectra due to the enhanced quinoidal character. The crystallographic data indicate that Se‐containing molecules exhibit more planar conjugate skeleton and thus lead to the improvement of carrier mobility. When blended with a polymer donor PBDB‐TF, ASe‐1‐, ASe‐2‐, and ASe‐3‐based organic photovoltaic (OPV) cells obtain power conversion efficiencies of 12.7%, 11.0%, and 10.4%, respectively. This work provides a comprehensive study of the application of Se substitution in designing low bandgap nfEAs for efficient OPV cells.

Near-Infrared Acceptors with Imide-Containing End Groups for Organic Solar Cells.

Near-infrared electron acceptors for organic solar cells (OSCs) mostly contain electron-withdrawing 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (IC) end groups, which can be modified by but limited to phenyl, thienyl, and naphthyl units with halogenated, methyl, and methyloxy substitution. In this work, we employed an imide-containing unit to construct a new IC end group, based on which a series of new electron acceptors were synthesized. The strong electron-deficient nature of imide units enables the new acceptors to show efficient intramolecular charge transfer and hence red-shifted absorption spectra compared to their IC counterparts. These new electron acceptors were applied to OSCs, providing efficiencies of over 17% with a low voltage loss of 0.52 eV. These results demonstrate that the new imide-containing end groups are promising fragments for the construction of near-infrared electron acceptors for high-performance OSCs.

The Radical Anion and Dianion of Benzo[3,4]cyclobuta[1,2-b]phenazine.

We present the reduction of two azaacenes (a benzo-[3,4]cyclobuta[1,2-b]phenazine and a benzo[3,4]cyclobuta[1,2-b]naphtho[2,3-i]phenazine derivative), featuring a single cyclobutadiene unit, to their radical anions and dianions. The reduced species were produced using potassium naphthalenide in the presence of 18-crown-6 in THF. Crystal structures of the reduced representatives were obtained and their optoelectronic properties evaluated. Charging these 4n Hückel systems gives dianionic 4n + 2 π-electron systems with increased antiaromaticity, according to NICS(1.7)zz calculations, featuring unusually red-shifted absorption spectra.

Counterion Control and the Spectral Signatures of Polarons, Coupled Polarons, and Bipolarons in Doped P3HT Films

AbstractWhen an electron is removed from a conjugated polymer, such as poly(3‐hexylthiophene‐2,5‐diyl) (P3HT), the remaining hole and associated change in the polymer backbone structure from aromatic to quinoidal are referred to as a polaron. Bipolarons are created by removing the unpaired electron from an already‐oxidized polymer segment. In electrochemically‐doped P3HT films, polarons, and bipolarons are readily observed, but in chemically‐doped P3HT films, bipolarons rarely form. This is explained by studying the effects of counterion position on the formation of polarons, strongly coupled polarons, and bipolarons using both spectroscopic and X‐ray diffraction experiments and time‐dependent density functional theory calculations. The counterion positions control whether two polarons spin‐pair to form a bipolaron or whether they strongly couple without spin‐pairing are found. When two counterions lie close to the same polymer segment, bipolarons can form, with an absorption spectrum that is blueshifted from that of a single polaron. Otherwise, polarons at high concentrations do not spin‐pair, but instead J‐couple, leading to a redshifted absorption spectrum. The counterion location needed for bipolaron formation is accompanied by a loss of polymer crystallinity. These results explain the observed formation order of single polarons, coupled single polarons, and singlet bipolarons in electrochemically‐ and chemically‐doped conjugated polymers.

Synthesis and Unexpected Optical Properties of Ionic Phosphorus Heterocycles with P-Regulated Noncovalent Interactions.

Optoelectronic properties of organic chromophores (OCPs) are to a large extent dictated by the chemical structures. Herein, we synthesized a new series of ionic phosphorus(P)-heteropines via the methylation of the P(III) center. Our studies revealed that methylation is highly dependent on the P(III) environments (NPN, NPC, and CPC), in which adjacent nitrogen atoms greatly withdraw electron density of the P(III) center. The observation of noncovalent interactions between solvent molecules and the molecular backbones of the related P-heterocycle in the single crystal structure implied tunable molecular conformations. Different from the red-shifted absorption and emission spectra of ionic P-OCPs induced by either decreased lowest unoccupied molecular orbital (LUMO) or intramolecular charge transfer (ICT) state in previous studies, current ionic P-heterocycles exhibit blue-shifted absorption and emission spectra compared to the nonionic counterparts. Our experimental and theoretical studies suggest that the unexpected photophysical characters are probably due to the counter-anion induced structure twisting via intermolecular noncovalent interactions between NH-indole and O(OTf), and/or strong intermolecular O···F bonding between O(MI) and F(OTf). Our studies also revealed that the P-environments (NPN, NPC, and CPC) conjunctly impact the photophysical properties of the ionic P-heteropines. Overall, the fact that the P-environment-regulated noncovalent interactions induce the rich structure dynamics and photophysics offers us with a new and effective strategy to fine-tune the optical properties of OCPs.

Selenophene-Containing Small-Molecule Donor with a Medium Band Gap Enables High-Efficiency Ternary Organic Solar Cells.

To construct efficient donor:donor:acceptor (D1:D2:A)-type ternary devices, two new selenophene-containing small-molecule (SM) donors named FSBTSeEHR and FSBTSeHR have been designed and synthesized that show broader and red-shifted absorption spectra than the thiophene analogues. With the introduction of SM donors into the D18:CH-6F host system, enhanced light harvesting and charge transport were achieved, benefiting from more complementary absorptions and cascaded energy levels. Furthermore, the doping of the SM donor could effectively modulate the micromorphology and enable a more suitable phase separation size in the active layer. After systematic optimization, the FSBTSeEHR-based ternary organic solar cell (TOSC) exhibited an excellent power conversion efficiency (PCE) of 18.02% with a high open-circuit voltage (Voc) of 0.905 V, short-circuit current density (Jsc) of 26.41 mA cm-2, and fill factor (FF) of 0.754. By contrast, the FSBTSeHR counterpart showed a superior efficiency of 18.55% due to the higher Jsc (26.91 mA cm-2) and FF (0.761). The outstanding PCEs of D1:D2:A-type TOSCs based on our SM donors, FSBTSeEHR and FSBTSeHR, are significantly higher than those of the corresponding binary host system (16.86%) and among the highest values reported to date. This work demonstrates that D1:D2:A-type TOSCs have tremendous potential to achieve superior performances through elaborate design of the SM donor guest and reasonable combination of D and A ingredients.

First principles study of the effect of (Mg, C) doping and Zn vacancies on the carrier activity, lifetime, visible light effect, and oxidation–reduction reaction of ZnO(0 0 1) monolayers

At present, some progress has been made in the study of Mg doping on the photocatalytic performance of ZnO monolayers. However, few studies on the effects of C impurities, Mg doping, and Zn vacancy coexistence on the electronic structure and photocatalytic performance of ZnO monolayers have been conducted. The preparation of ZnO through metal organic chemical vapor deposition growth technology inevitably generates C impurities, which are difficult to remove. To solve such problems, we investigated the effects of Mg doping and the coexistence of C impurities and Zn vacancies on the electronic structure and the photocatalysis of ZnO monolayers with a generalized gradient approximation plane-wave ultrasoft pseudopotential method based on the framework of density-generalized functional theory. Results showed that all doped systems had negative formation energy under O-rich conditions, indicating that the systems easily formed. The cohesion energy of Zn33CiCZnMgO36(Ci1−/2+/3+/4+,CZn2+) monolayers was relatively large, and the systems were stable. The absorption spectra of the doped systems red-shifted in a wavelength range of 425–800 nm compared with the absorption spectrum of the undoped Zn36O36 monolayer system. All doped systems were able to react with water to produce H2 and O2 at pH of 0 or 7. The Zn34CiCOMgO35 (Ci1−,CO2−) monolayer exhibited the strongest activity, the best absorption spectrum red shift, the smallest work function, the longest carrier lifetime, and the best HER ability. The Zn34CiCOMgO35 (Ci1−,CO2−) monolayer was considered a strong candidate for photocatalytic hydrogen production. Overall, this study has a theoretical reference value for the design and preparation of novel photocatalytic functional materials.

Effects of Sm and VZn in different valence states on the magnetic property, carrier lifetime, electric dipole moment, visible light, and redox reaction of ZnO:Hi under biaxial strain

This work uses the first principle to calculate the effects of the coexistence of different valence states of Sm and VZn on the photocatalytic and magnetic performance of ZnO containing interstitial H under strain. The result shows that the magnetic properties of Zn34Sm3+O36(VZn0/2−) and Zn34Sm3+HiO36(VZn0/2−) systems originate from the mixed-coupled double exchange of electron orbital of Sm-4f, Zn-4s, and O-2p. The state of Sm-4f and Zn-4s in Zn34Sm2+O36(VZn0/2−), Zn34Sm2+/3+HiO36(VZn0), and Zn34Sm2+HiO36(VZn2−) systems has independent single-ion magnetic characteristics. Based on the photocatalytic performance, the Zn34Sm3+HiO36(VZn2−) system has a long carrier lifetime, remarkably red shift of absorption spectrum, and redox ability when the compressive strain is −2%. The Zn34Sm3+HiO36(VZn2−) system is found to be a good photocatalyst when the compressive strain is −2%.