Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties
The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic proper...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Tang, Gang [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2021transfer abstract |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method - Xiao, Hong ELSEVIER, 2013, the international journal on the science and technology of electrochemical energy systems, New York, NY [u.a.] |
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| Übergeordnetes Werk: |
volume:514 ; year:2021 ; day:1 ; month:12 ; pages:0 |
| Links: |
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| DOI / URN: |
10.1016/j.jpowsour.2021.230546 |
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ELV055589774 |
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| 520 | |a The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. | ||
| 520 | |a The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. | ||
| 650 | 7 | |a Orbital engineering |2 Elsevier | |
| 650 | 7 | |a Orbital-energy splitting |2 Elsevier | |
| 650 | 7 | |a Ruddlesden-Popper layered perovskite |2 Elsevier | |
| 650 | 7 | |a Orbital-property relationship |2 Elsevier | |
| 700 | 1 | |a Wang, Vei |4 oth | |
| 700 | 1 | |a Zhang, Yajun |4 oth | |
| 700 | 1 | |a Ghosez, Philippe |4 oth | |
| 700 | 1 | |a Hong, Jiawang |4 oth | |
| 773 | 0 | 8 | |i Enthalten in |n Elsevier |a Xiao, Hong ELSEVIER |t Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method |d 2013 |d the international journal on the science and technology of electrochemical energy systems |g New York, NY [u.a.] |w (DE-627)ELV00098745X |
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10.1016/j.jpowsour.2021.230546 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001553.pica (DE-627)ELV055589774 (ELSEVIER)S0378-7753(21)01044-2 DE-627 ger DE-627 rakwb eng 690 VZ 50.92 bkl Tang, Gang verfasserin aut Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. Orbital engineering Elsevier Orbital-energy splitting Elsevier Ruddlesden-Popper layered perovskite Elsevier Orbital-property relationship Elsevier Wang, Vei oth Zhang, Yajun oth Ghosez, Philippe oth Hong, Jiawang oth Enthalten in Elsevier Xiao, Hong ELSEVIER Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method 2013 the international journal on the science and technology of electrochemical energy systems New York, NY [u.a.] (DE-627)ELV00098745X volume:514 year:2021 day:1 month:12 pages:0 https://doi.org/10.1016/j.jpowsour.2021.230546 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 50.92 Meerestechnik VZ AR 514 2021 1 1201 0 |
| spelling |
10.1016/j.jpowsour.2021.230546 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001553.pica (DE-627)ELV055589774 (ELSEVIER)S0378-7753(21)01044-2 DE-627 ger DE-627 rakwb eng 690 VZ 50.92 bkl Tang, Gang verfasserin aut Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. Orbital engineering Elsevier Orbital-energy splitting Elsevier Ruddlesden-Popper layered perovskite Elsevier Orbital-property relationship Elsevier Wang, Vei oth Zhang, Yajun oth Ghosez, Philippe oth Hong, Jiawang oth Enthalten in Elsevier Xiao, Hong ELSEVIER Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method 2013 the international journal on the science and technology of electrochemical energy systems New York, NY [u.a.] (DE-627)ELV00098745X volume:514 year:2021 day:1 month:12 pages:0 https://doi.org/10.1016/j.jpowsour.2021.230546 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 50.92 Meerestechnik VZ AR 514 2021 1 1201 0 |
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10.1016/j.jpowsour.2021.230546 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001553.pica (DE-627)ELV055589774 (ELSEVIER)S0378-7753(21)01044-2 DE-627 ger DE-627 rakwb eng 690 VZ 50.92 bkl Tang, Gang verfasserin aut Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. Orbital engineering Elsevier Orbital-energy splitting Elsevier Ruddlesden-Popper layered perovskite Elsevier Orbital-property relationship Elsevier Wang, Vei oth Zhang, Yajun oth Ghosez, Philippe oth Hong, Jiawang oth Enthalten in Elsevier Xiao, Hong ELSEVIER Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method 2013 the international journal on the science and technology of electrochemical energy systems New York, NY [u.a.] (DE-627)ELV00098745X volume:514 year:2021 day:1 month:12 pages:0 https://doi.org/10.1016/j.jpowsour.2021.230546 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 50.92 Meerestechnik VZ AR 514 2021 1 1201 0 |
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10.1016/j.jpowsour.2021.230546 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001553.pica (DE-627)ELV055589774 (ELSEVIER)S0378-7753(21)01044-2 DE-627 ger DE-627 rakwb eng 690 VZ 50.92 bkl Tang, Gang verfasserin aut Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. Orbital engineering Elsevier Orbital-energy splitting Elsevier Ruddlesden-Popper layered perovskite Elsevier Orbital-property relationship Elsevier Wang, Vei oth Zhang, Yajun oth Ghosez, Philippe oth Hong, Jiawang oth Enthalten in Elsevier Xiao, Hong ELSEVIER Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method 2013 the international journal on the science and technology of electrochemical energy systems New York, NY [u.a.] (DE-627)ELV00098745X volume:514 year:2021 day:1 month:12 pages:0 https://doi.org/10.1016/j.jpowsour.2021.230546 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 50.92 Meerestechnik VZ AR 514 2021 1 1201 0 |
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10.1016/j.jpowsour.2021.230546 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001553.pica (DE-627)ELV055589774 (ELSEVIER)S0378-7753(21)01044-2 DE-627 ger DE-627 rakwb eng 690 VZ 50.92 bkl Tang, Gang verfasserin aut Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. Orbital engineering Elsevier Orbital-energy splitting Elsevier Ruddlesden-Popper layered perovskite Elsevier Orbital-property relationship Elsevier Wang, Vei oth Zhang, Yajun oth Ghosez, Philippe oth Hong, Jiawang oth Enthalten in Elsevier Xiao, Hong ELSEVIER Numerical modeling of wave–current forces acting on horizontal cylinder of marine structures by VOF method 2013 the international journal on the science and technology of electrochemical energy systems New York, NY [u.a.] (DE-627)ELV00098745X volume:514 year:2021 day:1 month:12 pages:0 https://doi.org/10.1016/j.jpowsour.2021.230546 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 50.92 Meerestechnik VZ AR 514 2021 1 1201 0 |
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Orbital−energy splitting in Ruddlesden−Popper layered halide perovskites for tunable optoelectronic properties |
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The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. |
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The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. |
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The electronic orbital characteristics at the band edges play an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking Ruddlesden-Popper (RP) phase layered perovskites Cs n+1Ge n I n+1Cl 2n as examples, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, bandwidth) through a simple band structure parameter. Our results show that reducing the splitting energy |Δc| between the in-plane p x,y and out-of-plane p z orbitals at the conduction band minimum (CBM) can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with Δc is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edge. Therefore, we believe that our proposed orbital engineering approach will provide atomic-level guidance for understanding the performance limits of layered perovskite solar cells. |
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