QM Calculations Tutorial

Learn how to run quantum chemistry calculations using ORCA through OHMind’s QM agent.

Table of Contents

Overview

Difficulty: 🟡 Intermediate
Time: 45 minutes
Requirements: ORCA installed, OHMind_ORCA configured

In this tutorial, you will:

  1. Convert molecular structures to 3D coordinates
  2. Run geometry optimizations
  3. Calculate molecular properties (HOMO/LUMO, charges)
  4. Perform frequency calculations
  5. Analyze results for HEM applications

What is QM in OHMind?

OHMind integrates with ORCA, a powerful quantum chemistry package, to perform:

  • Geometry optimization - Find stable molecular structures
  • Single-point energy - Calculate electronic energy
  • Frequency calculations - Verify minima, get thermochemistry
  • Property calculations - HOMO/LUMO, charges, dipoles
  • Reactivity descriptors - For stability predictions

Prerequisites

ORCA Installation

Verify ORCA is installed and configured:

# Check ORCA path
echo $OHMind_ORCA
# Should show: /path/to/orca

# Test ORCA
$OHMind_ORCA --version

MPI Configuration (for parallel calculations)

# Check MPI path
echo $OHMind_MPI
# Should show: /path/to/mpi/bin

# Verify mpirun
$OHMind_MPI/mpirun --version

Workspace Setup

# Check QM workspace
echo $QM_WORK_DIR
# Should show: /path/to/workspace/ORCA

# Ensure directory exists and is writable
ls -la $QM_WORK_DIR

Start the Interface

cd OHMind
./start_OHMind_cli.sh

Part 1: Basic Calculations

Step 1.1: Convert SMILES to 3D Structure

Start by converting a SMILES string to 3D coordinates.

Prompt:

Convert this cation SMILES to 3D XYZ coordinates:
C[N+]1(C)CCCCC1

Use RDKit to generate a reasonable 3D structure.

Expected Output:

14
N-methylpiperidinium cation
C     0.000000     0.000000     0.000000
N     1.500000     0.000000     0.000000
...

Step 1.2: Single-Point Energy

Calculate the electronic energy of a structure.

Prompt:

For the cation SMILES "C[N+]1(C)CCCCC1":
1. Generate 3D coordinates
2. Run a single-point energy calculation using B3LYP/def2-SVP
3. Report the total energy in Hartree and kcal/mol

Expected Output:

Single-Point Energy Results:
- Method: B3LYP/def2-SVP
- Total Energy: -291.234567 Hartree
- Total Energy: -182,756.3 kcal/mol
- Calculation time: 45 seconds

Step 1.3: Quick Property Check

Get basic electronic properties.

Prompt:

For the cation "C[N+]1(C)CCCCC1", calculate:
1. HOMO energy
2. LUMO energy
3. HOMO-LUMO gap
4. Dipole moment

Use B3LYP/def2-SVP level of theory.

Expected Output:

Property Value Unit
HOMO -10.25 eV
LUMO -2.15 eV
Gap 8.10 eV
Dipole 3.45 Debye

Part 2: Geometry Optimization

Step 2.1: Basic Optimization

Optimize the molecular geometry to find the energy minimum.

Prompt:

Optimize the geometry of the cation "C[N+]1(C)CCCCC1":
- Method: B3LYP
- Basis set: def2-SVP
- Dispersion: D3BJ

Return the optimized coordinates and final energy.

What Happens:

  1. Initial 3D structure is generated
  2. ORCA input file is created
  3. Geometry optimization runs iteratively
  4. Converged structure is saved
  5. Final energy and coordinates are returned

Expected Duration: 5-15 minutes

Expected Output:

Geometry Optimization Complete:
- Converged in 12 cycles
- Final Energy: -291.456789 Hartree
- RMS Gradient: 0.000023
- Max Gradient: 0.000045

Optimized structure saved to: $QM_WORK_DIR/temp_xxx/input.xyz

Step 2.2: Verify Optimization

Confirm the optimization found a true minimum.

Prompt:

For the optimized geometry of "C[N+]1(C)CCCCC1", run a frequency 
calculation to verify it's a true minimum (no imaginary frequencies).

Report:
1. Number of imaginary frequencies
2. Lowest real frequency
3. Zero-point energy correction

Expected Output:

Frequency Analysis:
- Imaginary frequencies: 0 (confirmed minimum)
- Lowest frequency: 45.2 cm⁻¹
- Zero-point energy: 0.234567 Hartree
- Thermal correction to Gibbs free energy: 0.198765 Hartree

Step 2.3: Compare Conformers

Compare different conformations of a molecule.

Prompt:

For the cation "CC[N+](C)(CC)CC" (triethylmethylammonium):
1. Generate 3 different conformers
2. Optimize each at B3LYP/def2-SVP
3. Compare their energies
4. Identify the lowest energy conformer

Expected Output:

Conformer Energy (Hartree) Relative (kcal/mol)
1 -331.234567 0.0
2 -331.232456 1.3
3 -331.230123 2.8

Part 3: Property Calculations

Step 3.1: Charge Analysis

Calculate atomic charges for reactivity analysis.

Prompt:

For the optimized cation "C[N+]1(C)CCCCC1", perform charge analysis:
1. Mulliken charges
2. Hirshfeld charges
3. Identify the most positive atom (likely degradation site)

Expected Output:

Charge Analysis Results:

Mulliken Charges:
- N1: +0.45
- C2 (N-methyl): +0.12
- C3 (ring): -0.08
...

Hirshfeld Charges:
- N1: +0.38
- C2 (N-methyl): +0.08
...

Most positive atom: N1 (+0.45 Mulliken, +0.38 Hirshfeld)
This nitrogen is the likely site for nucleophilic attack.

Step 3.2: Frontier Orbital Analysis

Analyze HOMO and LUMO for reactivity.

Prompt:

For the cation "C[N+]1(C)CCCCC1", analyze the frontier orbitals:
1. HOMO and LUMO energies
2. HOMO-LUMO gap
3. Where is the LUMO localized? (important for nucleophilic attack)
4. What does this suggest about alkaline stability?

Expected Output:

Frontier Orbital Analysis:

Energies:
- HOMO: -10.25 eV
- LUMO: -2.15 eV
- Gap: 8.10 eV

LUMO Localization:
- Primarily on the nitrogen atom (45%)
- Secondary contribution from α-carbons (30%)

Stability Implications:
- Lower LUMO energy indicates higher susceptibility to nucleophilic attack
- LUMO localization on N suggests this is the primary degradation site
- Gap of 8.10 eV indicates moderate kinetic stability

Step 3.3: Alkaline Stability Descriptors

Calculate descriptors relevant to HEM stability.

Prompt:

For the cation "C[N+]1(C)CCCCC1", calculate alkaline stability descriptors:
1. LUMO energy (lower = less stable)
2. Electrophilicity index
3. Chemical hardness
4. Compare with a reference cation "C[N+](C)(C)C" (tetramethylammonium)

Expected Output:

Descriptor Piperidinium TMA Better
LUMO (eV) -2.15 -1.85 TMA
Electrophilicity 2.34 1.98 TMA
Hardness 4.05 4.52 TMA

Part 4: Advanced Calculations

Step 4.1: Proton Affinity

Calculate proton affinity for acidic groups.

Prompt:

Calculate the proton affinity of a sulfonic acid group in the context 
of an AEM. Use a model compound like methanesulfonic acid (CS(=O)(=O)O).

Report:
1. Gas-phase proton affinity
2. Estimated pKa

Expected Output:

Proton Affinity Results:

Gas Phase:
- Proton affinity: 315.2 kcal/mol
- Deprotonation energy: 342.1 kcal/mol

Solution Phase (estimated):
- pKa ≈ -2.6 (strong acid)

Interpretation:
Strong acid character indicates good proton donation capability.

Step 4.2: Binding Energy

Calculate ion binding energies.

Prompt:

Calculate the binding energy between a hydroxide ion (OH⁻) and 
the cation "C[N+]1(C)CCCCC1":
1. Optimize the ion pair
2. Calculate binding energy with BSSE correction
3. Compare with chloride (Cl⁻) binding

Expected Output:

Ion Binding Energy (kcal/mol) BSSE Correction
OH⁻ -85.3 2.1
Cl⁻ -72.1 1.8

Find transition states for degradation reactions.

Prompt:

Search for the transition state of hydroxide attack on the 
N-methyl group of "C[N+]1(C)CCCCC1" (SN2 mechanism).

Report:
1. Transition state geometry
2. Activation energy
3. Imaginary frequency (should be ~1)

Expected Output:

Transition State Results:

Geometry:
- C-N distance: 2.15 Å (breaking)
- C-O distance: 2.08 Å (forming)
- Angle: 172° (near linear)

Energetics:
- Activation energy: 28.5 kcal/mol
- Imaginary frequency: -456 cm⁻¹ (confirmed TS)

Interpretation:
Moderate activation barrier suggests reasonable kinetic stability.

Expected Outputs

File Locations

QM calculations create files in:

$QM_WORK_DIR/
├── temp_abc123/              # Per-job directory
│   ├── input.inp             # ORCA input file
│   ├── input.out             # ORCA output
│   ├── input.gbw             # Wavefunction file
│   ├── input.xyz             # Optimized geometry
│   ├── input_property.txt    # Extracted properties
│   └── input.hess            # Hessian (if frequencies)
└── results/                  # Archived results

Output File Contents

input.out - Main ORCA output containing:

  • Calculation settings
  • SCF convergence
  • Geometry optimization steps
  • Final energies
  • Orbital energies
  • Population analysis

input_property.txt - Extracted properties:

  • Total energy
  • HOMO/LUMO energies
  • Dipole moment
  • Charges

Interpreting Results

Property Good for HEM Concerning
LUMO energy > -2.0 eV < -3.0 eV
HOMO-LUMO gap > 8.0 eV < 6.0 eV
N charge < +0.4 > +0.5

Troubleshooting

Common Issues

Issue Cause Solution
“ORCA not found” Path not set Check $OHMind_ORCA
“SCF not converged” Difficult system Try different initial guess
“Optimization failed” Bad starting geometry Generate better conformer
“Imaginary frequency” Not a minimum Re-optimize from TS

Checking ORCA Output

Show me the last 50 lines of the ORCA output for my calculation.

Memory Issues

For large molecules, increase memory:

Run the calculation with 8 GB memory and 4 CPU cores.

Convergence Problems

The SCF didn't converge. Try the calculation again with:
1. Tighter integration grid
2. Different initial guess (SAD)
3. Level shifting

Next Steps

After completing this tutorial:

  1. Analyze with Multiwfn - Use wavefunction analysis for deeper insights
  2. Run MD simulations - Validate properties at finite temperature
  3. Compare candidates - Use QM to rank HEM optimization results

Suggested Follow-up Prompts

Take the wavefunction from my QM calculation and run a Multiwfn 
analysis to visualize the LUMO orbital and identify degradation sites.
For my top 5 HEM candidates, run QM calculations to compare their 
LUMO energies and rank them by predicted alkaline stability.

See Also


*Last updated: 2025-12-23 OHMind v1.0.0*

PolyAI Team
Copyright © 2009-2025 Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
Address: No. 5625, Renmin Street, Changchun, Jilin, China. Postal Code: 130022